Human exposure to chromium (Cr) via inhalation, ingestion, or dermal contact may pose toxicological concerns. This study assessed Cr levels in 850 surface soil samples and 106 wild mushrooms collected across Leicestershire, including the city of Leicester (England). ICP-MS analysis revealed Cr in 92.2% of 850 surface soil samples (median: 71.3 µg/g) and in 47.1% of 106 mushroom samples (median: 0.863 µg/g dw), with significantly higher values in urban areas, particularly in the southeast quadrant. Health risk assessments calculated for adults and children revealed that total hazard indices (HI) for Cr exposure through ingestion, dermal absorption, and inhalation were below 1 across all scenarios, indicating no immediate risk. Nevertheless, ingestion contributed the highest proportion of exposure (>75%), particularly in young children. Bioconcentration factors (BCFs) were calculated to assess Cr accumulation in fungi, revealing values well below 1, indicating low bioaccumulation potential. The findings suggest that while wild mushrooms reflect local soil contamination, they are not strong accumulators of chromium. This dual-matrix biomonitoring approach combining soils and fungi presents a valuable tool for mapping environmental contamination and identifying urban pollution hotspots. While estimated exposure values fall within acceptable thresholds, the absence of Cr(VI) speciation introduces uncertainty, underscoring the need for further research into its potential carcinogenicity. The findings underscore the importance of integrating environmental biomonitoring with risk communication strategies, particularly concerning mushroom foraging and urban gardening. This study supports continued environmental health surveillance in UK cities and the development of targeted public health interventions.