Some volcanic soils like andosols contain short-range order nanoclays (allophane) which build aggregates with a tortuous and fractal microstructure. The aim of the work was to study the influence of the microstructure and mesoporosity of the allophane aggregates on the pesticide chlordecone retention in soils. Our study shows that the allophane microstructure favors pollutants accumulation and sequestration in soils. We put forth the importance of the mesoporous microstructure of the allophane aggregates for pollutant trapping in andosols. We show that the soil contamination increases with the allophane content but also with the mesopore volume, the tortuosity, and the size of the fractal aggregate. Moreover, the pore structure of the allophane aggregates at nanoscale favors the pesticide retention. The fractal and tortuous aggregates of nanoparticles play the role of nanolabyrinths. It is suggested that chlordecone storage in allophanic soils could be the result of the low transport properties (permeability and diffusion) in the allophane aggregates. The poor accessibility to the pesticide trapped in the mesopore of allophane aggregates could explain the lower pollutant release in the environment.