LaLiga has filed a complaint to UEFA against Paris Saint-Germain over an alleged breach of financial fairplay rules.
In a statement released on Wednesday, LaLiga also said they had reported Manchester City to European football's governing body in April over the same allegations.
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LaLiga president Javier Tebas has accused Manchester City and PSG of "continuously breaching" financial fair play rules (FFP).
"LaLiga considers that these practices alter the ecosystem and the sustainability of football, harm all European clubs and leagues, and only serve to artificially inflate the market, with money not generated in football itself," the statement said.
Manchester City signed Borussia Dortmund forward Erling Haaland after paying his €60 million release clause earlier this month, while PSG renewed Kylian Mbappe's contract in May. Mbappe, who turned down a move to Real Madrid, was reportedly given a €150m bonus to remain in Paris while Haaland's deal, including salary and agent fees, could reportedly exceed £250m.
Tebas recently said that "no one believes" PSG's and City's figures.
"LaLiga understands that the irregular financing of these clubs is carried out, either through direct injections of money or through sponsorship and other contracts that do not correspond to market conditions or make economic sense," the league statement added.
LaLiga will also file a lawsuit against PSG in France, Switzerland and before the European Union.
It is not the first time LaLiga has acted against the state-owned football clubs.
In 2018, PSG were cleared of breaking UEFA's FFP rules while City was temporarily banned from the Champions League for breaching FFP regulations in 2020 but the punishment was overturned by Court of Arbitration for Sport (CAS) upon appeal.