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The first Double (1966–76)

The club appointed physiotherapist Bertie Mee as Wright's successor, a move that brought surprise to some, not least Mee himself. Nevertheless, Mee's appointment brought a brief period of glory. Arsenal's youth team had won the FA Youth Cup in 1966, and talented attacking players such as Charlie George, John Radford and Ray Kennedy graduated to the first team. Mee complemented this attacking ability with some more experienced heads; captain Frank McLintock at centre half marshalled a strong defence, while the hard-tackling Peter Storey filled the vital defensive midfield position. The team showed early signs of promise, reaching two successive League Cup finals in 1968 and 1969. Both times the Gunners went home empty-handed; the first to Don Revie's Leeds United 1-0; the second was an infamous upset – Arsenal losing 3-1 to Third Division side Swindon Town.

That season was not a total disaster for Arsenal; they had also finished fourth, which won them a place in Europe, and led to the club collecting their first silverware in seventeen years and their first European trophy, the 1970 Inter-Cities Fairs Cup. Arsenal beat Ajax in the semi-finals, and then staged a famous comeback against Anderlecht in the final. Arsenal were 3-0 down after 74 minutes of the first leg, but Ray Kennedy got a late away goal to give the Gunners a glimmer of hope; in the second leg in front of a packed Highbury, Arsenal won 3-0 with goals from John Radford, Eddie Kelly and Jon Sammels, to win the tie 4-3 on aggregate.

The highlight of this period was the club's first FA Cup and League Double win in 1970-71. Arsenal had started poorly, losing 5-0 to Stoke City in September. They recovered to put a strong run-in to the title in a tight race with Leeds United. Arsenal were pushed all the way to the title, and needed to beat deadly rivals Tottenham Hotspur at White Hart Lane on the last day of the season to overtake Leeds; they did just that, winning 1-0 thanks to a goal by Ray Kennedy. Five days later, Arsenal beat Liverpool 2-1 at Wembley; Arsenal went 1-0 down early in extra time, before substitute Eddie Kelly's equaliser, and then Charlie George scored the winner.

The Double proved to a premature high point of a decade characterised by a string of near-misses. Despite signing World Cup winner Alan Ball in the close season, Arsenal began 1971-72 badly, losing three matches in August, and were forced to play catch-up for the rest of the season, ultimately finishing fifth. Their debut in the European Cup started encouragingly, but they were knocked out in the quarter-finals by a Johann Cruyff-inspired Ajax playing at the very top of their game. Arsenal also reached the FA Cup final for the second year in a row; this time they lost 1-0 to Leeds United in an ill-disciplined and at times ugly match.

Arsenal finished as First Division runners-up in 1972-73, but within a year the Double-winning side had been broken up, and Mee was unable to build a new team in its place. The club's form declined sharply, finishing 16th in 1974-75 and 17th in 1975-76, their lowest in more than forty years, which prompted Mee's resignation. Tottenham manager Terry Neill, a former Arsenal player, was appointed in his place, even though he had never got Spurs anywhere beyond mid-table.