The content of heavy metals in honey is indicative of natural or anthropogenic pollution and has therefore been proposed as a feasible bioindicator for arsenic contamination in different regions of Chile. Total arsenic (t-As) and inorganic As (i-As) concentrations were determined in 227 samples of honey harvested during the years 2007, 2008, and 2009 in the areas of San Pedro de Atacama, Atacama, Chiloé, and Futaleufú, with the last town located 156 km from the Chaitén Volcano (latest eruption in 2008). These analyses were conducted using an atomic absorption spectrophotometer coupled with a hydride generator. In the honey samples, the concentrations of t-As ranged from 2.2 to 171.9 μg kg-1, and the i-As concentrations ranged from none detected (ND) to 24.6 μg kg-1, with the area of San Pedro de Atacama having the highest As concentrations. The samples of honey from Futaleufú showed higher As concentrations after the eruption of the Chaitén Volcano in 2008. This study demonstrates that As pollution in honey may originate from both natural and anthropogenic sources. The results indicate that it is appropriate to use honey as a bioindicator of environmental pollution. In addition, the consumption of the honey studied herein does not pose any health hazards to the consumer due to its As content.