The enigmatic Cambrian animal chancelloriids were discovered in a wide range of taphonomic settings; however, preservation of biomineralized sclerite microstructure was solely known from secondarily phosphatized skeletal remains. Here, we investigate a uniquely pyritized chancelloriid from the lower Cambrian Guojiaba Formation in southern Shaanxi Province, China, using a combination of advanced analytic techniques. Results of the energy dispersive spectroscopy (EDS), X-Ray Fluorescence (XRF), and Raman spectrum show that the sclerites and scleritomes are preserved as pyritized internal moulds with a calcitic outer layer. The outer layer enveloping the internal moulds likely represents the recrystallized counterpart of the original biomineralized sclerite wall. Distinctive fibrous microstructures are discovered in the sclerites, which echo the features seen in the phosphatized fossils of chancelloriids. The typical microstructure, along with the recrystallized calcite, corroborate the interpretation that chancelloriid sclerites were originally constructed by fibrous aragonite. The stability of the microstructure and mineral composition in both carbonate and siliciclastic backgrounds indicate that chancelloriids were adapted to exploit aragonitic fibres to build their skeletons regardless of the change of their living environments.