But the former first minister of Scotland stopped short of saying his successor, who he accuses of breaking the ministerial code, should stand down, saying that was a judgement for others.
During a highly-anticipated appearance before a Scottish parliament inquiry, the man who led the SNP for 20 years claimed Scotland’s current leadership had failed.
He also said there had been a “calculated and deliberate suppression of key evidence” to the committee.
And he alleged that Scottish government documents had been improperly withheld from the courts, in what he described as an “obstruction of justice”.
The list of those he said should resign or consider their position included the Scottish government’s permanent secretary, its chief law officer, Peter Murrell, the chief executive of the SNP who is also married to Ms Sturgeon, and the first minister’s chief of staff.
He was giving evidence just days after he accused a number of former SNP allies of a “malicious” effort to remove him from public life.
Watch: Nicola Sturgeon broke ministerial code, Salmond tells inquiry
MSPs are investigating the Scottish government’s handling of harassment allegations against Mr Salmond, which saw him awarded £512,000.
Scottish ministers were ordered to pay his legal fees after the Court of Session found the Scottish government’s investigation was “tainted by apparent bias” after it emerged the investigating officer had prior contact with two of the women who made complaints.
But Mr Salmond told the Holyrood committee they had been asked to do their job “with both hands tied behind its back and a blindfold on”.
He added: “Scotland hasn’t failed, its leadership has failed.
“The importance of this inquiry is for each and everyone of us to help put this right.”
Hours after Ms Sturgeon denied the identity of one of those who complained about Mr Salmond had been revealed, her predecessor suggested that was not true.
Mr Salmond said the name had been revealed to to Geoff Aberdein, his former chief of staff, and told MSPs there were three other people “who know that to be true”.
Yesterday Ms Sturgeon said: “To the very best of my knowledge, I do not think that happened.”
Mr Salmond also alleged there had been an “obstruction of justice” as he said government documents had been wrongly withheld from the courts.
He also said that if Ms Sturgeon had been aware that her government was about to lose the judicial review of his case, and had proceeded anyway, that would mean the first minister had breached the ministerial code.
The legal advice received by the Scottish government has not been published.
But Mr Salmond faced questions about his own behaviour when one of the members of the committee, Lib Dem MSP Alex Cole-Hamilton asked him: “Of the behaviours that you have admitted to, some of which are appalling, are you sorry?”
Mr Salmond replied: “Over the last three years there have been two court cases, two judges and a jury and I’m resting on the process.”
The former first minister had initially been due to give his evidence earlier this week.
But at the eleventh hour, he dramatically refused to appear amid an extraordinary row over a written submission he made to the committee.
The documents had been published by the Scottish parliament on its website.
But in a shock development, the submission was later removed and part of the evidence redacted.
It was then republished on the website, despite the original document being in the public domain for at least 16 hours.
The row was prompted by an intervention from the Crown Office, which oversees the prosecution of crime in Scotland and which expressed concerns over Mr Salmond’s submission.
The committee will quiz Ms Sturgeon on her version of events next week.