A new class of hydrogelators based on synthetic self-assembling N-terminally Boc-protected tripeptides has been developed. A series of five tripeptides have been synthesized to study their self-assembling behavior in aqueous medium. Three of them form thermoreversible translucent gels at basic pH (pH 11.5–13.5). These hydrogels were characterized by FT-IR spectroscopy, circular dichroism (CD), small angle X-ray diffraction analysis (SAXRD), field-emission scanning electron microscopic (FE-SEM), transmission electron microscopic (TEM) and atomic force microscopic (AFM) studies. These hydrogels can be potentially utilized for the treatment of waste-water and the organic dyes (Rhodamine B, Reactive Blue 4 and Direct Red 80) that are widely used in textile industries can be efficiently removed. Moreover, peptide gelators can be recovered very easily just by changing the pH of the medium.