Tanneries, among India’s earliest industries, historically used chromium (Cr) in leather and vegetable tanning, leading to unsuitable effluent discharge on land and in nearby water bodies. This research investigates chromium dispersion and accumulation in environmental and biological samples from the vicinity of closed tanneries in the Sembattu region, Tiruchirappalli district, South India. The study reveals chromium in sediment and biological samples but not in water samples. Sediment from S3 showed higher Cr concentration (132.65 ± 7.48 µg/g), with paddy straw 1 (18.72 ± 1.17 µg/g) and neem tree bark 3 (15.03 ± 1.04 µg/g) exhibiting higher plant concentrations. Among animals, cow dung 1 (143.93 ± 1.32 µg/g) and cow dung 5 (37.74 ± 1.28 µg/g) recorded higher concentrations. Geoaccumulation index (Igeo) values suggest “Uncontaminated-to-moderately contaminated” levels. The investigation reports permissible chromium concentrations in the Sembattu tannery area, yet groundwater salt levels exceed drinking water standards. The study highlights tanneries’ historical impact, stressing the need for increased awareness, strategic water management, and prudent land use planning. Future priorities include continuous monitoring, targeted remediation, community engagement, innovative research, and robust policy enforcement for sustainable environmental protection and resource management.