1,1-Dimethylsilacyclobutane, abbreviated as DMSCB, was investigated by Fourier transform microwave spectroscopy, by paying special attention to two types of large-amplitude motions in the molecule: two-top internal rotation and four-membered ring puckering and also to the coupling between the two. In order to clarify the unique feature of the internal dynamics in DMSCB in detail, two independent approaches were employed, one being a combination of a standard two-top theory of internal rotation and an established theory of ring puckering and the other a theory of large-amplitude motions developed by Hougen and his collaborators. In accordance with predictions by the two approaches based on symmetry consideration, the observed rotational spectra were found split into eight (or six when AE/ EA lines were not resolved) components, which were assigned to the two-top states of AA, AE, EA, and EE symmetry, each being further split by puckering into two: the symmetric and antisymmetric states. The analyses by two approaches gave spectroscopic results, which were in good agreement with each other. The spectroscopic data on the normal species, combined with those on Si and C isotopic species, yielded molecular structure parameters including the puckering angle (the dihedral angle between the CSiC and CCC planes) of 28.64° or 30.26° (two possible sets). The splitting between the two lowest puckering states was determined to be 11.90(22) MHz, which led, with the equilibrium puckering angle, to the potential barrier to puckering of 395.3 or 347.0 cm −1 for the two sets, respectively, which was slightly lower than the value 440 cm −1 in a “parent” molecule: silacylcobutane. The first-order terms of the coupling between CH 3 internal rotation and overall rotation were converted to the barrier to internal rotation of 567.8 and 505.1 cm −1 in the AE (two methyl groups rotating in the same direction, as viewed from Si) and EA (two methyl groups rotating in the opposite direction) states, respectively, which corresponded to the torsional frequencies of 154 and 144 cm −1, at variance with the Raman data of 177 and 172 cm −1, previously reported in literature.