Shallow littoral areas in lakes are productive and highly diverse ecotonal zones, providing habitats for both invertebrate and vertebrate species. We developed a Bayesian modeling framework to elucidate the relationships between environmental drivers (lake typology, habitat, water chemistry, and latitude) and taxon richness, abundance, as well as the content of polyunsaturated fatty acids (PUFAs) in littoral macroinvertebrate communities in 95 boreal lakes. PUFAs, particularly arachidonic acid (ARA), eicosapentaenoic acid (EPA), and docosahexaenoic acid (DHA), are critical micronutrients to maintain normal physiological functions in consumers. Lake typology was a significant predictor for PUFA content in the invertebrate assemblages, which was connected to taxon richness and/or abundance. Benthic communities in large humus-poor or nutrient-rich lakes displayed higher abundance, taxon richness, and more PUFA-rich taxa, whereas those in medium- and large-sized humic (color 30–90 mg Pt/L) and humus-rich lakes (color >90 mg Pt/L) were characterized by decreased abundance and subsequently low PUFA content. The abundance, taxon richness, and nutritional quality of the communities were also strongly related to latitude. Lakes with lower pH were characterized by lower benthic invertebrate diversity and low frequency of taxa with high somatic EPA and DHA content. The complexity of littoral habitats dominated by various macrophyte assemblages creates an environment that favors higher benthic abundance and increased presence of taxonomic groups with high PUFA content. Nutritional quality of benthic invertebrates for upper trophic levels can be modulated by a complex interplay between external stressors and abiotic factors that typically shape the structure of littoral benthic communities.