Changes in penguin populations on the Antarctic Peninsula have been linked to several environmental factors, but the potentially devastating impact of volcanic activity has not been considered. Here we use detailed biogeochemical analyses to track past penguin colony change over the last 8,500 years on Ardley Island, home to one of the Antarctic Peninsula’s largest breeding populations of gentoo penguins. The first sustained penguin colony was established on Ardley Island c. 6,700 years ago, pre-dating sub-fossil evidence of Peninsula-wide occupation by c. 1,000 years. The colony experienced five population maxima during the Holocene. Overall, we find no consistent relationships with local-regional atmospheric and ocean temperatures or sea-ice conditions, although the colony population maximum, c. 4,000–3,000 years ago, corresponds with regionally elevated temperatures. Instead, at least three of the five phases of penguin colony expansion were abruptly ended by large eruptions from the Deception Island volcano, resulting in near-complete local extinction of the colony, with, on average, 400–800 years required for sustainable recovery.