Contamination in coastal zones is an increasing problem that adversely affects biological diversity and the functioning of coastal ecosystems. Sediment is an important compartment of these zones since large quantities of diverse contaminants can accumulate there. Whole-sediment toxicity assays are of increasing importance, and several assay methods using mainly invertebrates have been developed. However, an important part of the benthic community, the microphytobenthos (represented principally by benthic diatoms and cyanobacteria), has surprisingly been neglected. Recently, comprehensive studies have been conducted using benthic marine microalgae with the object of establishing a toxicity assay method for sediment samples. The main results published to date in the literature and obtained by our own team have been compiled and are discussed in this review. The value and feasibility of using certain organisms of the microphytobenthos group in ecotoxicology studies are also discussed, and a sediment quality guideline based on multivariate procedure has been derived from data obtained in previous studies. Finally, future perspectives for research in this field are discussed.