"For 10 months, China has been paying Tariffs to the U.S. of 25% on 50 Billion Dollars of High Tech, and 10% on 200 Billion Dollars of other goods", Mr. Trump said.
Trump's tweet was an about-face from his recent comments that talks were progressing, with people familiar with the negotiations saying that the administration expected to announce a deal on Friday, following another round of talks this week in Washington.
The U.S. already imposes a 10 percent tariff on $200 billion of goods and a 25 percent tariff on $50 billion of tech products.
Trump has threatened to increase those tariffs before but has pushed back plans to raise them twice.
Trump's announcement comes ahead of another round of talks between USA and Chinese officials in Washington scheduled for this week.
Mr. Trump said on Sunday that his tariffs have had little impact on product costs in the United States and have been "mostly borne by China", an argument most economists dispute.
Trump and the Chinese president will decide after the negotiations this week whether they'll meet to sign off on a pact.
In the announcement on Twitter, Trump said that talks to secure a trade deal with China are continuing, but are moving "too slowly".
That follows talks in April in Beijing that US Treasury Secretary Steven Mnuchin called "productive".
As recently as last week, the U.S. had depicted the trade talks as going well.
"Nobody in the business community likes the tariffs", he said.
As a candidate for the presidency, Trump raged repeatedly about alleged Chinese perfidy - so much so that a video mashup of him spitting out the word "China" went viral and collected more than 15 million views on Youtube.com.
Despite Mnuchin's more upbeat interpretation of the last negotiating round, Pillsbury said he assumed Trump's tweet came after a more sobering update from U.S. Trade Representative Robert Lighthizer, including information that China had walked back from some things to which it had previously agreed. He has railed against America's trade deficit in goods China, which swelled previous year to record $419 billion.