Capital's loss of its perch was due less to its performance than a remarkable gain by Heart, which Chrysalis chief executive Phil Riley put down to investment in refreshing and marketing the station.
Capital's share of listening fell 0.1 percentage points over the quarter to 6.1%, while Heart increased its share from 5.3% to 7%.
Emap's Magic 105.4FM remains on Capital's heels with a 6% share, down from 6.1%. It attracted a record 1.73m listeners, adding 133,000.
All of the three increased the number of listeners they reach, in Heart's case by 14.9%.
Nationally, commercial stations again had to contend with a strong BBC. Radio 1, Radio 2 and Radio Five Live all grew their reach and share of listening.
Radio 1 went from 9.93m to 9.96m listeners and its share climbed from 8.2% to 8.4%. Radio 2 was up from 13.31m to 13.33m listeners and its share inched up from 16.4% to 16.5%.
Radio 4 fell back, losing 144,000 listeners to 9.26m and losing share from 11.5% to 11.4%. Five Live, on the other hand, added 153,000 listeners to 6.13m and grew its share from 4.3% to 4.6%.
Five Live's rival TalkSPORT performed well, adding nearly 500,000 listeners to reach 2.48m, and growing its share from 1.6% to 1.9%.
Back in London, concentration of listening among the top three saw less-listened to stations such as BBC London, Capital Gold, Choice, LBC and Xfm lose share.
However, there were other winners. Virgin London AM/FM grew its share from 3.3% to 3.7% and GMG Radio's Jazz FM, which was allowed by Ofcom to change its format in favour of soul and R'n'B, was boosted from 1.7% to 2.8%. Dance music station Kiss was unchanged at 3.9%.
Capital's breakfast show DJ Johnny Vaughan was also a winner, attracting 108,000 more listeners than in the last quarter. The total of 1,238,000 listeners for his show was rivalled only by Jono and Harriet on Heart, who achieved 972,000, with an extra 124,000 listeners tuned in for the pair's swansong quarter, ahead of Jamie Theakston's arrival as a replacement for Jono.
Nationally, GWR's Classic FM's share fell from 4.4% to 4.1% and its reach fell from 6.2m to 5.98m.
Capital, which is about to merge with GWR to form GCap Media, saw its local Century network grow its reach slightly and hold steady with a 1.6% share.
Emap's Kiss network lost almost 200,000 listeners, at 2.19m, but still grew its share from 1.1% to 1.2%. Its Magic network kept a 2.1% share while adding 183,000 listeners to reach 2.94m.
Chrysalis's Heart network had a good quarter, seeing its share increase by 1.8% to 2.2% as well as climbing to more than 3m listeners. However, its Galaxy network lost listeners and its share declined from 1.9% to 1.7%.
Virgin Radio, which potential buyer Lord Alli accused of being underinvested in by its owner SMG, lost 41,000 listeners to 2.42m but grew its share from 1.4% to 1.5%.
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