The Congress said the prime minister should apologise for demonetisation as it had inflicted "misery" on the people and dealt a "body blow" to the economy.
Congress senior spokesperson Anand Sharma said none of the measures that Modi had promised with the ban on high-value currency notes, put into effect in November last year, had been realised.
He also said in the last six quarters under Modi, the GDP growth sank from 9.2 per cent to 5.7 per cent.
The CPI-M termed demonetisation as a "money laundering exercise that helped convert black money into white" at the expense of people and asked prime minister to come clean on it and fix accountability as the move "failed" to achieve its objectives.
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The AAP said demonetisation broke the backbone of the country's economy and lashed out at the Reserve Bank of India for "lying" to the nation about the total amount of Rs 500 and Rs 1,000 notes in circulation before the drive.
Congress incharge of communications Randeep Surjewala drew a parallel of Modi with 14th-century monarch Muhammad bin Tughlaq for his decision to demonetise and demanded his resignation for "misleading" the people of the country.
"PM Modiji will go down in history alongside Mohammad- Bin-Tuglaq for Demonetisation Scam. If morality has a place, he should consider to quit," Surjewala said on Twitter.
He also said that Modi made a disaster of demonetisation due to which India's economy was wrecked and asked what gains did note ban bring to the country.
"GDP growth slows from over 8 pc to 5.7 pc yet those living in glass houses of demonetisation disaster remain oblivious in their ivory towers.
"In last 6 quarters, the economy under Modiji sank from 9.2 pc to 5.7 pc! This is by new method of calculation! Is this demonetisation success formula?" Surjewala asked.
Sharma stressed it was the prime minister's "direct responsibility" as it was his personal decision to implement note ban.
Sharma alleged demonetisation had led to a GDP loss of Rs 2.25 lakh crore.
He said Modi had promised to unearth black money and end corruption, terror funding and counterfeit currency.
None of the promises made by him while announcing the decision had come true, he said.
The opposition attack came after the Reserve Bank said in its annual report yesterday that banks had received Rs 15.28 lakh crore or 99 per cent of the invalidated currency.
AAP leader Sanjay Singh said, "We have been saying since day one that demonetisation is one of the biggest scams in independent India which has broken the backbone of the country's economy. The prime minister should apologise to the nation."
Another Left party, the CPI, stated that RBI's annual report for 2016-17, released yesterday, raises several questions, given there is no information on quantum of black money unearthed due to demonetisation, and also attributed the falling GDP to the note-ban.
Sharma wondered what the note ban decision had achieved as 99 per cent of the money had been returned, and accused the prime minister of "changing the narrative" on the issue.
"The prime minister made a sensational announcement on November 8 that unleashed financial anarchy and economic chaos in the country. The Reserve Bank figures yesterday exposed the falsehood propagated by the government," he said.
Training his guns on Modi, Sharma said he kept "changing his narrative and kept pace with a species called the chameleon, which keeps changing its colours".
He added that Modi's ministers, too, had a "direct responsibility".
Sharma accused Modi of defaming his own people before the world. Had this happened in any other country, the PM would not be in office, he added.
He asked the prime minister to explain his Independence Day speech where he mentioned that Rs 3 lakh crore of black money had been unearthed and challenged him to make public the list of companies and individuals whose undeclared money it was.