Arsenobetaine, an organo-arsenic compound known to be non-toxic, occurs ubiquitously in marine animals. To elucidate the food hygiene safety of the degradation products of arsenobetaine formed on cooking, arsenicals generated by roasting the muscles of the starspotted shark Mustelus manazo and of the red crayfish Panulirus longipes femoristriga were investigated. As a result, both muscle types were found to contain the tetramethylarsonium ion, which is reported to show a higher acute toxicity than dimethylarsinic acid (cacodylic acid) or methanearsonic acid. As a minor compound, arsenate was also detected in the muscle of M. manazo.