While the standard model of particle physics does not include free particles with fractional charge, experimental searches have not ruled out their existence. We report results from the Cryogenic Dark Matter Search (CDMS II) experiment that give the first direct-detection limits for cosmogenically produced relativistic particles with electric charge lower than e=6. A search for tracks in the six stacked detectors of each of two of the CDMS II towers finds no candidates, thereby excluding new parameter space for particles with electric charges between e=6 and e=200. DOI: 10.1103/PhysRevLett.114.111302 PACS numbers: 95.35.+d, 14.80.-j Fractionally charged particles are a well-known feature of the standard model (SM) of particle physics; quarks and antiquarks possess either AE2=3 or AE1=3 of the electron charge e. Because of the nature of the strong interaction, however, these particles are bound inside hadrons. Free particles with smaller charges are viable in extensions of the PRL 114, 111302 (2015) P H Y S I C A L