Cops had began excavating an area of Saddleworth last week after an author came forward claiming he found a skull.
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Russell Edwards told officers he had discovered a fragment of skull and an upper jaw with teeth, sparking a week-long search.
It was hoped the huge breakthrough could finally crack the riddle that has plagued police and his family for nearly 60 years.
But police called off their search for little Keith on Friday after finding no evidence of human remains.
And Keith’s brother Alan Bennett, 66, has now said he had been left with a “feeling of anger and pain”.
In a lengthy post on social media, he wrote: “I’m just left with a feeling of utter contempt for him and his actions and I know the rest of Keith’s family feel the same, along with anger and pain.”
He added: “Will he apologise for the anguish, anger, hurt and distress caused by his thoughtless publicity-seeking actions?”
In the angry post Mr Bennett said: “Why would there only be a fragment of jaw bone left of Keith, considering the condition of the other victims that were found?”
He continued: “Does he always have a camera crew and photographer with him? Or was it just by pure chance and coincidence that they were with him on his supposed find?
“What makes him think that a team of highly trained professional forensic archaeologists, scene of crime officers, a botanist, a facial features expert, lab technicians, another team of officers walking the moor both in front and behind of his supposed find searching the ground, drone operatives and the complete professionalism and care to conduct a search thoroughly could not find what he is supposed to have found?”
Tragically, Keith’s mum Winnie went to the grave without ever being able to bury her son.
Ian Brady and Myra Hindley snatched Keith on June 16, 1964, as he made his way to his grandmother’s house.
He was strangled and buried on Saddleworth Moor by the depraved duo but his body has never been found.
A spokesman for Mr Edwards said he “totally understands” Mr Bennett’s frustration and anguish, reports The Mirror.
He added: “However, he remains convinced that he has found the true location of the grave and is commissioning further scientific analysis of his evidence.
“Until he has concluded his ongoing research, he feels it would not be productive to continue debating the issues in public.”
Edwards told police the skull is believed to belong to a child aged around 12 with a child’s upper jaw with a full set of teeth.
Detectives were also focusing on a sample of material believed to be clothing that was buried 3ft under the remains.
How evil couple horrified nation with Moors murders
On July 12, 1963, Brady told Hindley he wanted to “commit his perfect murder”.
Hindley would often lure the children in before driving them to Saddleworth Moor or the pair’s home.
Brady would then kill them often by throat slashing or strangling.
Four of the five victims were sexually assaulted as well as murdered.
They were also beaten, abused and gagged and made to pose for photographs.
The five victims were:
- Pauline Reade, 16
- John Kilbride, 12
- Keith Bennett, 12
- Lesley Ann Downey, 10
- Edward Evans, 17
The reign of terror came to an end in 1965 when Brady invited Hindley’s brother-in-law and friend, David Smith, round to their home.
The monster then murdered Edward Evans – striking him fourteen times with a hatchet before finishing the job by strangling him – while Smith looked on in horror.
Under the pretence of helping them hide the body, Smith left and phoned the police next morning and directed them to Brady’s address.
On October 7, 1965, Superintendent Bob Talbot of the Cheshire Police arrived at the back door of 16 Wardle Brook Avenue and arrested the killer after discovering Edward’s body.
Over the course of the next few weeks, officers unearthed more evidence linking the couple to unsolved disappearances.
A huge search operation involving 150 officers was launched and on October 16, they found an arm bone sticking out of the ground belonging to Lesley Ann.
They discovered the badly decomposed body of Kilbride five days later.
On June 30, 1987, the body of Pauline Reade was found buried 3 feet below the ground after Brady finally admitted to her murder.
The author explained to police he had recovered a fruit stone, clothing material, hair and “what he described as decaying body tissue”.
After viewing a photograph and the samples provided, the area was secured by detectives so a forensic archaeological excavation could be carried out.
She added: “The excavation and examination at the site is complete and, to reiterate, we have found no evidence that this is the burial location of Keith Bennett.”
DCI Cheryl Hughes said the search for Keith “will not be closed until we have found the answers his family have deserved for so many years.”
Keith was lured into a van by Hindley, who drove him to a lay-by on the Moor.
Brady then took him away to sexually assault and murder him while Hindley kept watch.
Keith’s family have fought ever since to recover the little lad’s remains.
After he was transferred from prison to maximum-security hospital Ashworth in November 1985, Brady confessed to Keith’s murder in an interview.
A search was carried out on the moors a year later, with Hindley joining officers in 1986 and Brady in 1987.
But Keith’s body was never found and it is became a grisly secret Brady took to the grave.