Atriums, in most conditions, are considered the heart of buildings, the main spaces where different functions and activities are held. Nowadays, various atrium designs are incorporated in the building, varying from pyramidal to barrel vault. Therefore, it is of great importance to study the basic characteristics of sound fields in such spaces and their related materials. This research aims to determine the effect of various skylight geometry configurations on the atrium’s acoustical performance. Next, an acoustical performance evaluation of the effect of skylight materials was performed by using computer simulation. Four selected atriums with different types of skylight geometries modeling and respective materials, i.e., glass, polycarbonate, and acrylic, have been used in this acoustical simulation. From the results, it can be concluded that an atrium with a pyramidal skylight provides a better reverberation time for music purposes. In contrast, all atriums’ models’ speech transmission index values were almost identical. However, no significant acoustical performance can be found in different used materials. The result also indicates that the shape of the atrium has a higher effect on the acoustical performance than the different materials used.