Photoluminescence (PL), up-conversion PL (UCPL), and phosphorescence are three kinds of phenomena common to light-emitting materials, but it is very difficult to observe all of them simultaneously when they are derived from a single material at room temperature. For the first time, triple-mode emission (that is, PL, UCPL, and room temperature phosphorescence (RTP)) is reported, which relies on a composite of the luminescent carbon dots (CDs) prepared from m-phenylenediamine and poly(vinyl alcohol) (PVA). Moreover, the CDs-PVA aqueous dispersion is nearly colorless and demonstrates promise as a triple-mode emission ink in the field of advanced anti-counterfeiting.