Typically two-dimensional (2D) free-standing crystals exhibit properties that differ from those of their 3D counterparts [1]. Currently, however, there are relatively few such atomically layered solids [2-5]. Here, we report on 2D nanosheets, composed of a few Ti3C2 layers and conical scrolls, produced by the room temperature exfoliation of Ti3AlC2 in hydrofluoric acid. The large elastic moduli predicted by ab initio simulation, and the possibility of varying their surface chemistries (herein they are terminated by hydroxyl and/or fluorine groups) render these nanosheets attractive as polymer composite fillers. Theory also predicts that their bandgap can be tuned by varying their surface terminations. The good conductivity and ductility of the treated powders suggest uses in Li-ion batteries, pseudo- capacitors, and other electronic applications. Since Ti3AlC2 is a member of a 60+ group of layered ternary carbides and nitrides known as the MAX phases, this discovery opens a door to the synthesis of a large number of other 2D crystals.