Cassava-groundnut intercropping is not a common practice among smallholder farmers in Sierra Leone even though both crops are well suited for intercropping. On-farm trials were conducted in three locations (Bai Largor, Bassah, and Njala Kanima) in the Moyamba district during the 2021 cropping season to investigate the efficacy of cassava-groundnut intercropping for increasing crop productivity and soil organic carbon stock on smallholder farms in the Moyamba district, Southern Sierra Leone. The experimental design was a randomized complete block design in three replications with treatments of sole groundnut, sole cassava and cassava-groundnut intercropping. Data on the yield and yield components of cassava and groundnut were analysed using the PROC MIXED procedure of SAS 9.4 and means were compared using the standard error of difference (SED). The above-ground biomass, number of roots per plant, and fresh root yield of cassava were not significantly (p > 0.05) affected by the cassava-based cropping system. Averaged across locations, intercropping cassava with groundnut decreased the above-ground biomass, the number of roots per plant, and fresh root yield of cassava by 17%, 11%, and 17%, respectively. The above-ground biomass, number of pods per plant and fresh pod yield of groundnut were significantly (p < 0.05) affected by the groundnut-based cropping system. Averaged across locations, intercropping groundnut with cassava decreased the aboveground biomass, the number of pods per plant, and fresh pod yield of groundnut by 33%, 15%, and 31%, respectively. The cassava-groundnut intercropping treatment had favourable