AbstractSamarium (Sm) is a rare‐earth element recently included in the list of critical elements due to its vital role in emerging new technologies. With an increasing demand for Sm, microbial bioremediation may provide a cost‐effective and a more ecologically responsible alternative to remove and recover Sm. We capitalized on a previously selected Chlamydomonas reinhardtii strain tolerant to Sm (1.33 × 10−4 M) and acidic pH and carried out settling selection to increase the Sm uptake performance. We observed a rapid response to selection in terms of cellular phenotype. Cellular size decreased and circularity increased in a stepwise manner with every cycle of selection. After four cycles of selection, the derived CSm4 strain was significantly smaller and was capable of sequestrating 41% more Sm per cell (1.7 × 10−05 ± 1.7 × 10−06 ng) and twice as much Sm in terms of wet biomass (4.0 ± 0.4 mg Sm · g−1) compared to the ancestral candidate strain. The majority (~70%) of the Sm was bioaccumulated intracellularly, near acidocalcisomes or autophagic vacuoles as per TEM‐EDX microanalyses. However, Sm analyses suggest a stronger response toward bioabsorption resulting from settling selection. Despite working with Sm and pH‐tolerant strains, we observed an effect on fitness and photosynthesis inhibition when the strains were grown with Sm. Our results clearly show that phenotypic selection, such as settling selection, can significantly enhance Sm uptake. Laboratory selection of microalgae for rare‐earth metal bioaccumulation and sorption can be a promising biotechnological approach.