On 16 December 2015,[5] Pooley announced that she would be returning temporarily to cycling, seeking to qualify to represent Great Britain at the 2016 Summer Olympics in Rio, as she felt the unusually mountainous time trial course on offer played to her strengths.

[24] She won her first major stage race in May, the final edition of the Tour de l'Aude,[25] the longest-running event on the UCI women's calendar.

[28] In March 2011, Pooley won the one-day Trofeo Alfredo Binda World Cup race for a second time, again after a lengthy lone breakaway.

She broke her collarbone in training on 12 April so was unable to defend her Flèche Wallonne title and did not race again until the women's invitational time trial at the Tour of California on 20 May,[29] in which she placed fifth.

Later in the year, however, she won the hilly Tour de l'Ardèche stage race in France and finished second to Marianne Vos in the Giro d'Italia Femminile, both achievements that she would repeat in 2012.

Pooley took a step back from pro-racing when she signed for the long-established, but non-UCI registered, Swiss-based Bigla Cycling Team for the 2013 season[32] in order to concentrate on completing her PhD in geotechnical engineering.

[40] Pooley made a return to competitive cycling in October 2015 when she competed at the Chrono des Nations time trial, where she finished sixth.

[41] In December 2015 she announced that she would aim to compete for Team GB in the 2016 Summer Olympics in Rio de Janeiro after being approached by British Cycling's technical director Shane Sutton, who had studied the Olympic road racing courses and felt that Pooley would have a good chance of winning a medal in the time trial and of helping Lizzie Armitstead to win the road race.

[42] Pooley made her first appearance in a mass start road race for two years in April 2016 for the British national team at the Women's Tour de Yorkshire, where she helped teammate Alice Barnes to fourth place.

[44] At the Olympics, Pooley rode in the service of Armitstead in the road race, whilst in the time trial she finished 14th, just over two minutes down on winner Kristen Armstrong.

The event takes the form of a Le Mans style start as 500+ smartly-dressed competitors have to unfold their bikes and completed eight lap circuit around St James Park.

[47] Her ascent (and descent) covered 129.8 km, and beat the previous female Everesting record of 9 hours 08:31 set by Hannah Rhodes on the Kirkstone Pass in England on 8 June 2020.

In November 2022, she raced for the Swiss national team at the World Mountain and Trail Running Championships in Thailand, finishing 11th in the 80 km event.

[62] Pooley has lived in or near Zürich in Switzerland since 2006, and in December 2013 completed her doctorate in geotechnical engineering at ETH Zurich, supervised by Sarah Springman, a former British triathlete who is a vice-president of the International Triathlon Union.