The Canberra-based outfit, who reached the 2013 final and the semi-finals in the last two seasons, are among the pre-season favourites to win the newly expanded competition.
Scrumhalf Nic White and fullback Jesse Mogg have headed to France but otherwise they have retained a squad rich in test talent for the new campaign.
At the end of the season, however, totemic captain Stephen Moore is off to Queensland, flyhalf Matt Toomua to Leicester, winger Joe Tomane to France, while flanker David Pocock looks set to take a sabbatical.
"We've spoken about this a little bit, it is a last chance," Larkham told Reuters this week.
"This group's been together for four years now, this really is the last opportunity as a group to achieve something and they're highly motivated.
"There is a bit of expectation, and we want to achieve something as a group but the best way to do that is not focus on the finals, but on winning the first game."
Larkham, of course, was a standout in the team's golden era, steering the Brumbies backline from flyhalf as they reached four finals in five years and won the title twice.
WORLD CUP LIFT
It has not escaped his notice that their 2001 and 2004 triumphs came in the wake of the Wallabies reaching the 1999 and 2003 World Cup finals -- a feat they matched in England last year.
"I've been thinking about that a lot over the last month," the pensive and quietly spoken 41-year-old said.
"I think there is a flow-on effect to the Super Rugby sides. It was a good journey for the boys who were involved and I think we surprised a few people.
"Rugby's at a peak in Australia at the moment and the boys are certainly riding on that."
The Brumbies had the best defensive record in Super Rugby in 2015, conceding just 21 tries in 16 games, but after losing a few tight matches last year, Larkham knows that might not be enough to take the final couple of steps to the title.
"That's obviously something we're very proud of but we can't rest on that," he added.
"The biggest thing we have to improve is our attacking game, we've been tinkering with our attacking style, not only from set piece but also from multi-phase, so that'll be biggest change you'll see."
Larkham, who is also out of contract at the end of the year, was part of the Wallabies' journey to October's World Cup final as attack coach under Michael Cheika.
Seen by many as Cheika's long-term successor as head coach, Larkham said he was still "weighing up" whether he could continue combining the role with his duties at the Brumbies.
And whatever happens in the new season, which starts for the Brumbies next Friday with a rematch of last year's semi-final against the Wellington Hurricanes, he looks unlikely to be leaving Australia's capital any time soon.
"I'm certainly keen to stay with the Brumbies," he said.
(Editing by John O'Brien)
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