Polylactic acid (PLA) is the most common polymeric material in the 3D printing industry but degrades under harsh environmental conditions such as under exposure to sunlight, high-temperatures, water, soil, and bacteria. An understanding of degradation phenomena of PLA materials is critical to manufacturing robust products by using 3D printing technologies. The objective of this study is to evaluate four machine learning algorithms to classify the degree of thermal degradation of heat-treated PLA materials based on Fourier transform infrared spectroscopy (FTIR) data. In this study, 3D printed PLA specimens were subjected to high-temperatures for extended periods of time to simulate thermal degradation and subsequently examined by using two types of FTIR spectrometers: desktop and portable spectrometers. Classifiers created by multi-class logistic regression and multi-class neural networks were appropriate prediction models for these datasets.