The Russian billionaire who bought a 14.6 per cent share in Arsenal last month has upped his investment vehicle's share in the club by a further 6.4 per cent.
Red and White Holdings, which is co-owned by Alisher Usmanov and his investment partner Farhad Moshiri, has announced it has bought more shares in the north London club.
It now holds a 21 per cent stake in Arsenal, making it the second-biggest shareholder after Danny Fiszman, who has a 24 per cent share, a statement released to the London stock exchanged confirmed.
Former Gunners vice-chairman David Dein was made chairman of Red and White Holdings last month when the original stake was purchased for £75 million.
Dein left the Arsenal board in acrimonious circumstances in April after his fellow directors reportedly refused to back his plan to seek foreign investment in the club.
Manager Arsene Wenger was seen as a close ally of Dein and the latter's departure prompted fears among many of the club's fans about the Frenchman's future at the Emirates Stadium.
But Wenger has since committed himself to Arsenal until 2010, increasing speculation that Dein is set to lead a takeover bid for the club to pave the way for a reunion of the two men at the Gunners' helm.
Towards the end of last season, the main shareholders at the club pledged not to sell their shares for at least 12 months.
Arsenal are due to announce their latest financial figures next week, with analysts predicting the 2006 move to the 60,000-capacity Emirates Stadium from Highbury will see a huge boost in profits.