This study spatially analysed the relation between mercury (Hg) content in soil and Hg in rock fragment for the purpose of assessing natural soil Hg contribution compared with Hg from human inputs. We present the Hg content of 318 soil and rock fragment samples from 11 islands distributed into two Spanish archipelagos (the volcanic Canary Islands [Canaries] and the Mediterranean Balearic [Balearic] islands). Assumedly both are located far enough away from continental Hg sources to be able to minimise the effects of diffuse pollution. Physical and chemical soil properties were also specified for the samples. Hg contents were significantly greater in the Balearic limestone soils (61 μg kg(-1)) than in the volcanic soils of the Canaries (33 μg kg(-1)). Hg levels were also greater in topsoil than in rocky fragments, especially on the Balearics. The soil-to-rock ratios varied between 1 and 30. Interestingly, the highest topsoil-to-rock Hg ratio (>16 ×) was found in the vicinity of a coal-fired power plant in Majorca, whereas no similar areas in the Canary archipelago were identified.