Abstract: Precision of the best molecular spectroscopy is currently orders of magnitude behind atomic ion spectroscopy, owing primarily to challenges in molecular state preparation and readout. Applications of improved molecular spectroscopy would include searches for time-variation of fundamental constants, parity violation studies, and searches for fundamental electric dipole moments. Our group at Northwestern University is developing the necessary tools to perform clock-quality spectroscopy on single trapped molecular ions. We are currently working with species having semi-closed electronic cycling transitions, so that optical pumping into the rotational ground state can be achieved by pulse-shaping of a resonant femtosecond laser. I will also describe a simple readout technique we are developing to map the internal molecular state onto a co-trapped atomic ion, using a pulsed radiation pressure force to excite secular motion.