The cubic polytype of silicon carbide is an interesting candidate for Micro-Electro-Mechanical-Systems (MEMS) applications due to its tremendous physico-chemical properties. The recent development of multi-stacked Si/SiC heterostructures has demonstrated the possibility to obtain a (110)-oriented 3C–SiC membrane on a 3C–SiC pseudo-substrate, using a silicon layer grown by low pressure chemical vapor deposition as a sacrificial one. However, the (110) orientation of the 3C–SiC membrane led to a facetted and rough surface which could hamper its use for the development of new MEMS devices. Then, in this contribution, an optimized growth process is used to improve the surface quality of the 3C–SiC membrane. The progress relies on the mastering of a (111) orientation for the SiC film, resulting in a smooth surface. Such an optimized structure could be the starting point for the achievement of new MEMS devices in medical or harsh environment applications.