Inland valleys are becoming increasingly important agricultural production areas for rural households in sub-Saharan Africa due to their relative high and secure water availability and soil fertility. In addition, inland valleys are important as water buffer and biodiversity hot spots and they provide local communities with forest, forage, and fishing resources. As different inland-valley ecosystem functions may conflict with agricultural objectives, indiscriminate development should be avoided. This study aims to analyze the diversity of inland valleys in Sierra Leone and to develop guidelines for more precise interventions. Land use, biophysical and socio-economic data were analyzed on 257 inland valleys using spatial and multivariate techniques. Five cluster groups of inland valleys were identified: (i) semi-permanently flooded with high soil organic carbon (4.2%) and moderate available phosphorus (10.2 ppm), mostly under natural vegetation; (ii) semi-permanently flooded with low soil organic carbon (1.5%) and very low available phosphorus (3.1 ppm), abandoned by farmers; (iii) seasonally flooded with moderate soil organic carbon (3.1%) and low available phosphorus (8.3 ppm), used for rainfed rice and off-season vegetables produced without fertilizer application for household consumption and market; (iv) well drained with moderate soil organic carbon (3.8%) and moderate available phosphorus (10.0 ppm), used for rainfed rice and off-season vegetables produced with fertilizer application for household consumption and market; and (v) well drained with moderate soil organic carbon (3.6%) and moderate available phosphorus (11 ppm), used for household consumption without fertilizer application. Soil organic carbon, available phosphorus, hydrological regime, physical accessibility and market opportunity were the major factors affecting agricultural intensification of inland valleys. Opening up the areas in which inland valleys occur through improved roads and markets, and better water control through drainage infrastructures along with an integrated nutrient management would promote the sustainable agricultural use of inland valleys.