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The discovery of new families of exfoliatable 2D crystals that have diversesets of electronic, optical, and spin-orbit coupling properties, enables therealization of unique physical phenomena in these few-atom thick buildingblocks and in proximity to other materials. Herein, using NaSn2As2 as a modelsystem, we demonstrate that layered Zintl phases having the stoichiometryATt2Pn2 (A = Group 1 or 2 element, Tt = Group 14 tetrel element and Pn = Group15 pnictogen element) and feature networks separated by van der Waals gaps canbe readily exfoliated with both mechanical and liquid-phase methods. Weidentified the symmetries of the Raman active modes of the bulk crystals viapolarized Raman spectroscopy. The bulk and mechanically exfoliated NaSn2As2samples are resistant towards oxidation, with only the top surface oxidizing inambient conditions over a couple of days, while the liquid-exfoliated samplesoxidize much more quickly in ambient conditions. Employing angle-resolvedphotoemission spectroscopy (ARPES), density functional theory (DFT), andtransport on bulk and exfoliated samples, we show that NaSn2As2 is a highlyconducting 2D semimetal, with resistivities on the order of 10-6 {\Omega} m.Due to peculiarities in the band structure, the dominating p-type carriers atlow temperature are nearly compensated by the opening of n-type conductionchannels as temperature increases. This work further expands the family ofexfoliatable 2D materials to layered van der Waals Zintl phases, opening upopportunities in electronics and spintronics.

NaSn2As2: An Exfoliatable Layered van der Waals Zintl Phase