Wastewater treatment plants (WWTPs) have been identified as significant point sources of microlitter particles (MPs) released into the environment. Simultaneously, they play a crucial role in effectively removing a substantial amount of MPs originated from domestic and industrial activities. This study evaluates the presence and chemical composition of MPs within the range of 5 mm to 25 µm in effluents from three WWTPs in the Canary Islands, each undergoing distinct treatment processes: pretreatment (PRET), activated sludge (AS), and membrane bioreactor (MBR) over an eight-month period. The concentrations of MPs exhibited substantial variations in the three effluent samples: 7461.50 ± 3843.87 MP/L in PRET, 32.71 ± 19.55 MP/L in AS, and 9.53 ± 5.21 MP/L in MBR. The predominant forms of MPs were fragments (58–66%) and fibers (27–33%), with the most prevalent size class being within the range of 150–25 µm. The mass concentrations of plastics, analyzed through pyrolysis gas chromatography–mass spectrometry (Pyr-GC/MS), were determined as 123.33 µg/L for PRET, 17 µg/L for AS, and 10 µg/L for MBR. This study revealed a diverse polymer profile, with polyvinyl chloride (PVC) and polyolefins (PE and PP) predominantly present. This work enhances our understanding of MP dynamics and provides a valuable reference for future assessments, aiding in the selection of effective removal technologies.