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The 25-year-old won seven major trophies in his four seasons at the Nou Camp, including the Champions League once and La Liga twice.
He said his father, Neymar Sr, wanted him to stay at Barcelona.
“I have won all that a player can win,” said Neymar, who will earn 45m euros (£40.7m) a year on a five-year deal.
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Writing on Instagram, he added: “I have conquered everything an athlete can conquer. I have lived unforgettable moments. But a player [me] needs challenges.
“And for the second time in my life, I’ll contradict my father.”
Wearing No. 10 for PSG, @neymarjr. Has a nice ring to it, don't you think?! 😃 pic.twitter.com/93EJArPYtk
— PSG English (@PSG_English) August 3, 2017
Neymar’s transfer smashes the previous record set when Paul Pogba returned to Manchester United from Juventus for £89m in August 2016.
His £782,000-a-week wages mean PSG’s total outlay is £400m.
The French side have called a news conference for 12:30 BST on Friday, and Neymar will be introduced to fans at PSG’s first game of the season against Amiens at Parc des Princes on Saturday.
PSG reached the last eight of the Champions League last season – knocked out by a Neymar-inspired Barcelona – and were beaten to the French title by Monaco.
Neymar said he has joined “one of the most ambitious clubs in Europe”.
“Paris St-Germain’s ambition attracted me to the club, along with the passion and the energy this brings,” he added.
There's just something special about seeing 'Neymar' on the back of a yellow shirt! 😍🇧🇷@PSG_inside #AllezParis #PSG #BemvindoNeymarJR pic.twitter.com/7L46fxY8WE
— Dugout (@Dugout) August 3, 2017
“I feel ready to take the challenge. I will do everything I can to help my new team-mates.”
A late snag?
After weeks of speculation, Neymar arrived at Barcelona’s training ground on Wednesday with his father and representative, and told the Spanish club he wanted to leave.
He was then given permission by Barca manager Ernesto Valverde to leave to “sort out his future”.
In Spain, a release clause can only be activated by a player buying himself out of his contract.
But when Neymar’s lawyers attempted to make the deposit on Thursday, La Liga officials rejected the payment. Further statements followed from all sides as the negotiations continued.
La Liga believes PSG are violating Uefa’s Financial Fair Play (FFP) rules and Barcelona previously said they would report PSG to European football’s governing body Uefa for an FFP breach.
PSG believes La Liga was acting unlawfully, while the French league (LFP) said it was “surprised” and urged its Spanish counterpart to “abide by the Fifa rules”.
Unable to get La Liga to take the payment, Neymar’s representatives paid the 222m euros (£200m) at Barca’s offices instead.
