Quantifying the changing patterns and determinants of material stocks (MS) is important for understanding the interplay between socioeconomic development and environment conservation, and for addressing the challenges in sustainable development. This paper conducts a MS accounting for 10 materials in 6 major infrastructures in Beijing, Tianjin and Shanghai, and probes into the driving factors behind the change within the 1978–2013 period through a logarithmic mean divisia index decomposition method. The results suggest that MS changes through a rapid enhancement in the 1980s, a steadily growth in the 1990s, and an acceleration after the 2000s. A relative decoupling phenomenon was detected in the development of economy and MS, which was largely caused by the decline of MS intensity. The policy implications include paying more attentions to the improvement of MS efficiency especially in buildings, substituting for less energy-intensive construction materials, controlling the extensive urban sprawl, and raising the population density.