We present Hubble Space Telescope WFC3/IR images of the Cassiopeia A supernova remnant that survey its high-velocity, S-rich debris in the NE jet and SW counterjet regions through [S III] lambda lambda 9069, 9531 and [S II] lambda lambda 10,287-10,370 line emissions. We identify nearly 3400 sulfur emitting knots concentrated in similar to 120 degrees wide opposing streams, almost triple the number previously known. The vast majority of these ejecta knots lie at projected distances well out ahead of the remnant's forward blast wave and main shell ejecta, extending to angular distance of 320 '' to the NE and 260 '' to the SW from the center of expansion. Such angular distances imply undecelerated ejecta knot transverse velocities of 15,600 and 12,700 km s(-1), respectively, assuming an explosion date approximate to 1670 AD and a distance of 3.4 kpc. Optical spectra of knots near the outermost tip of the NE ejecta stream show strong emission lines of S, Ca, and Ar. We estimate a total mass similar to 0.1 M-circle dot and a kinetic energy of at least similar to 1 x 10(50) erg for S-rich ejecta in the NE jet and SW counterjet. Although their broadness and kinetic energy argue against the Cas. A SN being a jet-induced explosion, the jets are kinematically and chemically distinct from the rest of the remnant. This may reflect an origin in a jet-like mechanism that accelerated interior material from a Si-, S-, Ar-, and Ca-rich region near the progenitor's core up through the mantle and H-, He-, N-, and O-rich outer layers with velocities that greatly exceeded that of the rapidly expanding photosphere.