In this work, calculations were made based on the MP2 method and 6-311++G(3df,3pd) basis set in order to study the formation mechanism of molecular clusters CH3CHO∙∙∙(HF)1≤n≤4 formed by acetaldehyde with hydrogen fluoride. By increasing the quantity of hydrogen fluoride molecules in the molecular clusters, the cluster's stability was ascertained. Proton transfer takes place between the molecules of hydrogen fluoride when the number of molecules in the cluster is more than four. Here, it was observed that the C=O bond length and hydrogen bond energy increase with increasing n. The vibrational frequencies corresponding to C-H that has been blue-shifted are shown to grow above around ~100 cm-1. This leads to a tight link among different structural factors.