Mr Moore described the trebling of tuition fees south of the Border as "the biggest, ugliest, most horrific thing in all of this . . . a car crash, a train wreck".
He told undercover reporters the move was "deeply damaging" to Lib Dems, who had promised to abolish fees.
He also said cutting child benefit for higher-rate taxpayers was "not a fair thing to do". Business Minister Ed Davey said he was "gobsmacked" by the decision, and Pensions Minister Steve Webb said he had written to George Osborne seeking changes to the policy.
The comments were published a day after Business Secretary Vince Cable was stripped of some responsibilities after he said he had "declared war" on Rupert Murdoch over his bid to secure full ownership of BSkyB.