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La Liga have filed complaints to UEFA regarding Manchester City and Paris Saint-Germain for "continuously breaching" financial fair play regulations.
The Spanish division made an initial complaint in April regarding Premier League champions City and has followed it up with another complaint about French giants PSG.
La Liga also cited conflict of interests regarding PSG president Nasser Al-Khelaifi, due to his role as European Club Association chairman and his role as the organisation's delegate to UEFA's executive committee.
In a statement, La Liga said their complaint was due to the fact that the clubs are "continuously breaching" FFP regulations and believe that "these practices alter the ecosystem and the sustainability of football" and "only serve to artificially inflate the market with money not generated in football itself."
The confirmation of the complaints falls after a big month for both clubs, with PSG confirming a new contract for star striker Kylian Mbappe prior to Real Madrid's Champions League success and City landing Erling Haaland from Borussia Dortmund – with both players previously heavily touted for a move to Spain.
Both City and PSG have previously been investigated for allegedly breaching FFP regulations, with both clubs fined in 2014 and having transfer spending limited – but a ruling to ban City from European competitions due to "serious breaches" was overturned by the Court of Arbitration for Sport after appeals from the English side.
PSG boast the two most expensive transfers of all-time with their captures of Mbappe from Monaco and Neymar from Barcelona in 2017, with the deal to sign the Brazilian costing €222 million.
Last year, City made Jack Grealish the most expensive Premier League transfer in history with a £100m transfer from Aston Villa.
Despite La Liga's complaints about the spending of the two clubs, Spanish sides dominate the list of the most expensive signings in football history with five of the top ten all seeing a Spanish side complete the signing.