Trump said in a tweet that the tech giant's search engine had "rigged" news story results to show mostly "bad" stories about him and other conservatives.
"Google search results for 'Trump News' shows only the viewing/reporting of Fake New Media," the president said.
"In other words, they have it RIGGED, for me & others, so that almost all stories & news is BAD. Fake CNN is prominent. Republican/Conservative & Fair Media is shut out."
Trump added: "Illegal? 96% of … results on 'Trump News' are from National Left-Wing Media, very dangerous. Google & others are suppressing voices of Conservatives and hiding information and news that is good. They are controlling what we can & cannot see. This is a very serious situation-will be addressed!"
Around 11 a.m. ET, Trump deleted the original tweets and reposted practically identical language.
"When users type queries into the Google Search bar, our goal is to make sure they receive the most relevant answers in a matter of seconds," a Google spokesperson said in a statement Tuesday.
"Search is not used to set a political agenda and we don't bias our results toward any political ideology. Every year, we issue hundreds of improvements to our algorithms to ensure they surface high-quality content in response to users' queries. We continually work to improve Google Search and we never rank search results to manipulate political sentiment."
Trump also praised the performance of the Nasdaq Compositeindex, which climbed above 8,000 points for the first time ever Monday.
Google's parent company Alphabet is a key driver of the Nasdaq's performance. The firm's shares were under pressure following Trump's comments, down around 0.5 percent.
Later Tuesday, Larry Kudlow, Trump's economic advisor, told Bloomberg that the White House is "looking into" whether Google suppresses positive articles about the president.
Some reports have suggested the president was referring to an unscientific report by conservative news website PJ Media, which claimed that 96 percent of Google search results for the word "Trump" showed left-leaning publications. The report places outlets including CNN, The Washington Post and The Guardian on the left of the political spectrum, while placing the likes of Fox News, the New York Post and the Daily Mail on the right.