State prosecutor Marilyn Mosby said the death of the 25-year-old black man was a homicide, and his arrest was illegal.
The charges range from second-degree murder to assault. Protesters cheered as she made the announcement.
Gray suffered fatal spinal injuries while in custody, sparking protests that turned violent.
"The findings of our comprehensive, thorough, and independent investigation coupled with the medical examiner's determination was a homicide... has led us to believe that we have probable cause to file criminal charges," Mrs Mosby told a news conference.
She said Mr Gray died as a result of injuries suffered while he was shackled inside a Baltimore police van, but not restrained by a seat belt - as he was legally required to be.
The six police officers were expected to turn themselves in to the Baltimore jail on Friday, the Baltimore sheriff's office said. The officers were suspended after Gray's death.
The driver of the van, Caesar Goodson, 45, faces the most serious charge, second-degree murder. Mr Goodson faces more than 30 years in prison if conviction.
The other officers face charges including involuntary manslaughter, assault and misconduct.
"To the people of Baltimore and the demonstrators across America, I heard your call for 'no justice, no peace'. Your peace is sincerely needed, as I work to deliver justice on behalf of this young man." Mrs Mosby said.
Mrs Mosby said that Gray was not carrying a switchblade as reported earlier by police, but a legal pocketknife.
The police union defended the officers and said they acted "diligently". The union called for an independent prosecutor, something Mosby said was not needed.
After Gray's funeral on Monday, riots broke out in sections of West Baltimore. About 200 people were arrested as more than 100 cars were set alight and 15 buildings destroyed.
Since then, the city and state officials deployed thousands of extra law enforcement officers and National Guard troops to keep the peace and enacted a citywide curfew.
Those measures have brought relative calm to Baltimore as thousands have taken part in nightly protests.
At North and Pennsylvania avenues, where the worst of the rioting took place on Monday, drivers honked their horns and passers-by cheered.
President Barack Obama responded to questions about the charges in Washington, saying the legal process should run its course.
"What I think the people of Baltimore want more than anything else is the truth," Mr Obama said.
Ciara Ford of Baltimore expressed surprise at the decision to prosecute.
"I'm ecstatic," she told the Associated Press. "I hope this can restore some peace."
Gray's death is the latest in a string of high-profile cases where black men have died after contact with the police.
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