In this paper, a framework of probabilistic-based mixture regression models (PMRM) is presented for multi-class alignment of liquid chromatography-mass spectrometry (LC-MS) data. The proposed framework performs the alignment in both time and measurement spaces of the LC-MS spectra. The expectation maximization (EM) algorithm is used to estimate the joint parameters of spline-based mixture regression models and prior transformation densities. The latter are incorporated to account for variability in time and measurement spaces of the data. As a proof of concept, the proposed method is applied to align a single-class replicate LC-MS spectra generated from proteins of lysed E.coli cells. Its performance is compared with the dynamic time warping (DTW) and continuous profile model (CPM) approaches.