As the world No.4, Murray is an obvious contender for medals in the singles event, which will be played at Wimbledon just three weeks after the end of the Championships, where the Scot will also be hoping to break his grand-slam duck.
Yet, as he is quick to tell you, Murray gets even more satisfaction from winning doubles matches with his brother than he does from big wins in singles, and the pair will be hoping to upset some of the bigger names next month. "I don't think it can get any better than that, really," Murray said yesterday at Wimbledon, dressed in official GB Team kit as he was announced as the first Briton on the Olympic tennis team.
"I know what it was like watching Jamie winning the mixed doubles here. I wasn't even playing and that was fairly emotional for me, so I can't imagine what it would be like to win an Olympic medal."
Though they enjoyed the overall experience of being at the Olympics in Beijing four years ago, the brothers lost in the second round and Murray admitted their shared room in the Olympic Village after-wards was "not a great place to be".
Watching the Murrays play together can be tough going, with neither wanting to let the other down. Doing it under the spotlight of a home Olympics, Murray said, might be even more emotional. "It's going to be tough," he said. "It's hard to explain unless you've maybe been in that position before. There's the pressure of playing for your country and then, obviously, having your brother on the court with you and you want to do well for him, as well. It can be tough.
"When I play doubles with Jamie, I want to do well. I put a lot of pressure on myself because I know it can help him and it's also his career, as well. To get the chance to play with him at an Olympics is going to be great but, at the same time, it is going to be fairly stressful. Hopefully, the doubles goes well, because, if it doesn't, then the singles will become a bit tougher."
Murray said he would relish the pressure of being involved in a home Games. "If you're not itching to get out there and perform, you're probably in the wrong job," he said. "That's what we train and prepare for. Everything I've seen and heard from all of the British athletes is that everyone is so excited for it.
"People have retired and come back because the Olympics is going to be in London, people have prolonged their career because it's going to be in London, so there's no reason why everyone shouldn't be excited."
Murray, so far, is the only player confirmed as part of Team GB, although he will also qualify to play with his brother in the doubles, while Colin Fleming and Ross Hutchins are hopeful of earning direct entry. Other players will have to wait until Thursday, when the International Tennis Federation announces the wild cards.
As host nation, Britain are in a strong position and Paul Hutchins, Team GB's tennis team leader, is optimistic they will be represented in all five events: men's singles and doubles, women's singles and doubles and mixed doubles, which is included in the programme for the first time.
Anne Keothavong, as British No.1, is in pole position for any wild cards awarded to Britain for the women's singles while Elena Baltacha, Heather Watson and Laura Robson are also contenders. Hutchins said: "We are hopeful that we will get a decent representation of British players. We put up a very strong case to the ITF via the BOA [British Olympic Association]."