The effect the material-built environments exert on people’s perception is vital for people’s wellbeing. However, the correlation between the material and the space is under-researched. The development of smart building technologies brings opportunities and challenges to explore this problem, no matter for the material type or for the study method. In this research, 18 indoor environments in two sizes covered by nine materials in VR are used to examine the influence of the materials on people’s perceptions. This research uses a preference survey as the primary data gathering tool. Statistical tests used are Kruskal-Wallis and Mann-Whitney. The results reveal that there is a significant difference in the preference level among the simple cubic indoor environments covered with different materials. The results also reveal that the change in size appears to influence the material preference level following a certain rule, but it can induce a significant effect on the preference level of only several specific materials. This study furthermore highlights that the results may be useful to extend the knowledge that designers and architects have of the perception to indoor environments and may propose a new idea for generating or improving a smart indoor environment.