Black carbon (BC) and total organic carbon (TOC) along with their relationship with organochlorine pesticides (OCPs) and polychlorinated biphenyls (PCBs) were assessed in Lesser Himalayan Region (LHR) in different altitudinal zones based on anthropogenic influence/source proximity under the scope of this study. Results revealed the concentrations of BC, TOC, OCPs and PCBs varied between 0.3 and 43.5 mg g− 1, 1.7–65.4 mg g− 1, 0.59–3.64 ng g− 1 and 0.01–1.31 ng g− 1, respectively. Spatial distribution trends have shown higher levels of OCPs and PCBs contamination near populated and urban areas along the altitude. It is implicated that upslope, short and long-range transport and local emission sources contribute to the contamination of different altitudinal zones of LHR. The relationship of BC and TOC with OCPs and PCBs was evaluated using principal component analysis (PCA) and Pearson correlation analysis that indicated higher sorptive influence of BC over TOC in distribution status of organochlorines in LHR. Further research is required to find relationship of BC and TOC in surface riverine sediments, particularly in aquatic systems along the altitude in mountain regions of the world.