The focus of this paper is the Neolithic of northwest Europe, where a rapid growth in population between ~5950 and ~5550 cal yr BP is followed by a decline that lasted until ~4950 cal yr BP. The timing of the increase in population density correlates with the local appearance of farming and is attributed to the advantageous effects of agriculture. However, the subsequent population decline has yet to be satisfactorily explained. One possible explanation is the reduction in yields in Neolithic cereal-based agriculture due to worsening climatic conditions. The suggestion of a correlation between Neolithic climate deterioration, agricultural productivity, and a decrease in population requires testing for northwestern Europe. Data for our analyses were collected during the Cultural Evolution of Neolithic Europe project. We assess the correlation between agricultural productivity and population densities in the Neolithic of northwest Europe by examining the changing frequencies of crop and weed taxa before, during and after the population “boom and bust.” We show that the period of population decline is coincidental with a decrease in cereal production linked to a shift towards less fertile soils.