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Boserup’s pioneering theory holds that rising population density can be accompanied by sustainable agricultural intensification. But can this positive relationship be sustained indefinitely, or are there conditions under which rising population density can lead to declining agricultural productivity? This study utilizes survey data on farm households in Kenya and soil samples on their main maize plots to assess whether Boserupian agricultural intensification is sustainable at high population densities. The study employs econometric estimation methods to assess the effect of land management practices and population density on soil quality and then determines the effect of soil quality on crop productivity. Results show evidence of endogenous sustainable agricultural intensification accompanied by improvements in soil quality and crop yields at low population densities. However, as population densities exceed roughly 600 persons/km2, we observe a deterioration in indicators of soil organic and reactive carbon, soil pH, and plant available phosphorous. Deterioration in soil quality leads to binding nutrient constraints associated with reduced crop yield response to inorganic fertilizer application that further reduces crop productivity. These results raise the specter of unsustainable forms of agricultural intensification associated with deteriorating soil capital, and point to the imperative of identifying and implementing effective strategies for increasing farmers’ use of sustainable land management practices in rural areas facing already high and rising population densities.