The analysis of microplastics (MP) becomes more difficult for smaller sizes, especially in complex matrices such as sediment of natural waters. In this work, we analyzed MPs in sediment using laser direct infrared (LDIR) imaging, a relatively new technique in environmental MP studies. Sediment samples were spiked with analytical surrogates (polyethylene spheres), and subjected to density separation, wet peroxide oxidation, calcite removal, and filtration. The extracted particles were coated on to a low-emissivity glass slide which was first examined on a stereomicroscope. Six slides (two sediment samples and four different blanks) were further analyzed using an Agilent LDIR system. Approximately 520 and 430 MP/g were found in the two samples, with diameter ranging 20-3,384 μm and 84% being smaller than 100 μm. The increase in particle count with decreasing particle sizes followed a power law curve, suggesting that a large portion of the smaller MPs was generated by the breakdown of larger plastic pieces. Major polymers found in this work included polyamide, polyester, polytetrafluoroethylene, and polyacetal. Most MPs were fragments, while beads and fiber were also found. In the two sediment samples, 14% and 46% of the total particles, respectively, were composed of non-plastic micro-sized particles, including natural polyamide, cellulose, chitin, rubber, and “unknown”. Challenges, potential biases, and uncertainties are discussed. This work is the first application of LDIR imaging on MPs in natural sediment.