The neurotoxin β-N-methylamino-l-alanine (BMAA) is naturally present in some microalgal species in the marine environment. The accumulation of BMAA has widely been observed in filter-feeding bivalves that are known to consume primary producers constituting the base of complex aquatic food webs. This study was performed to assess the occurrence of BMAA and isomers in mollusks collected from nine representative shellfish production areas located on the three French coasts (Channel, Atlantic and Mediterranean sites). The use of a highly selective and sensitive HILIC-MS/MS method, with D5DAB as internal standard, revealed the systematic detection of BMAA and DAB, in concentrations ranging from 0.20 to 6.7 μg g−1 dry weight of digestive gland tissues of mollusks. While we detected BMAA in four strains of diatoms in a previous study, here BMAA was only detected in one diatom species previously not investigated out of the 23 microalgal species examined (belonging to seven classes). The concentrations of BMAA and DAB in mussels and oysters were similar at different sampling locations and despite the high diversity of phytoplankton populations that mollusks feed on at these locations. Only small variations of BMAA and DAB levels were observed and these were not correlated to any of the phytoplankton species reported. Therefore, extensive research should be performed on both origin and metabolism of BMAA in shellfish. The levels observed in this study are similar to those found in other studies in France or elsewhere. A previous study had related such levels to a cluster of Amyotrophic Lateral Sclerosis in the South of France; hence the widespread occurrence of BMAA in shellfish from all coasts in France found in this study suggests the need for further epidemiological and toxicological studies to establish the levels that are relevant for a link between the consumption of BMAA-containing foodstuffs and neurodegenerative diseases.