Emerson was also a member of a record eight Davis Cup winning teams between 1959 and 1967.

1963 also saw Emerson capture his first French Championships singles title, beating Pierre Darmon in the final.

Emerson was the World No. 1 amateur player in 1964 and 1965 according to Lance Tingay of The Daily Telegraph and in 1967 according to Rex Bellamy. In 1965, he successfully defended his Australian and Wimbledon singles crowns. He was the heavy favourite to win Wimbledon again in 1966, but during his fourth round match he skidded while chasing the ball and crashed into the umpire's stand, injuring his shoulder. He still finished the match, but was unable to win.

Emerson's last major singles title came at the French Championships in 1967 – the year before the open era began. His 12 major singles titles stood as a men's record until 2000, when it was surpassed by Pete Sampras. Emerson signed a professional contract with the National Tennis League in early April 1968.

Although he exited the tournament circuit, Emerson did not retire. In the late 1970s, he served as a player/coach for the Boston Lobsters in World Team Tennis (WTT). He mostly played doubles with the Lobsters and often teamed with fellow Australian Tony Roche. In the 1978 season, the last season under the original iteration of World Team Tennis, Roy coached the Lobsters to the Eastern Division Championship and into the WTT Finals against the Los Angeles Strings. The final Lobster team that Emerson coached consisted of Tony Roche, Mike Estep (for part of the season), and Emerson himself as the male players.

Emerson's final Grand Slam doubles title was won in 1971 at Wimbledon (partnering Laver). His 16 Grand Slam doubles crowns were won with five different partners. From 1960–1965, he won six consecutive French Open men's doubles titles. Jack Kramer, the long-time tennis promoter and tennis great, writes in his 1979 autobiography that "Emerson was the best doubles player of all the moderns, very possibly the best forehand court player of all time. He was so quick he could cover everything. He had the perfect doubles shot, a backhand that dipped over the net and came in at the server's feet as he moved to the net. Gene Mako and Johnny van Ryn could hit a shot like that sometimes, but never so often nor as proficiently as Emerson."

Emerson's last top-20 ranking was in 1973, primarily owing to his winning his 105th and final career title at the Pacific Coast Championships in San Francisco. He defeated Roscoe Tanner, Arthur Ashe, and Björn Borg in the last three rounds of that tournament. Emerson played just a few tournaments through 1977. His last appearance was in the Gstaad, Switzerland tournament in 1983.

Emerson now resides in Newport Beach, California with his wife, Joy, and daughter, Heidi, and has a home in Gstaad where he holds a tennis clinic each summer. His son, Antony, was an All-American in tennis at Corona del Mar High School and the University of Southern California and played on the professional tour briefly. Roy and Antony won the United States Hard Court Father-and-Son title in 1978. Roy briefly coached promising juniors at East Lake Woodlands in Oldsmar, Florida. His students included Pat Cash, Kim Warwick, and Derek Damico.

Emerson was inducted into the International Tennis Hall of Fame in 1982 and the Sport Australia Hall of Fame in 1986. The main court for the Suisse Open Gstaad, a tournament which Emerson won five times and where he played his last match as a professional, is named Roy Emerson Arena in his honour.

In 2000 he was awarded the Australian Sports Medal, and in 2001 received the Centenary Medal.

The Roy Emerson trophy, which is awarded to the male champion at the Brisbane International, is named in his honour. In 2009 Emerson was inducted into the Queensland Sport Hall of Fame. He was honoured during the 2013 Australian Open at the Australian Open Legends' Lunch.

In 2014 Brisbane named new courts in Milton at Frew Park after Roy Emerson. The same year at Blackbutt, the Roy Emerson Museum was opened by Roy Emerson. On the 18 January 2017 a Statue of Roy Emerson was unveiled at the Blackbutt Museum.