Abstract The North American Nanohertz Observatory for Gravitational Waves (NANOGrav) project has the primary goal of detecting and characterizing low-frequency gravitational waves through high-precision pulsar timing. The mitigation of interstellar effects is crucial to achieve the necessary precision for gravitational wave detection. Effects like dispersion and scattering are stronger at lower observing frequencies, with the variation of these quantities over week–month timescales requiring high-cadence multifrequency observations for pulsar timing projects. In this work, we utilize the dual-frequency observing capability of the Giant Metrewave Radio Telescope (GMRT) and evaluate the potential decrease in dispersion measure (DM) uncertainties when combined with existing pulsar timing array data. We present the timing analysis for four millisecond pulsars observed with the GMRT simultaneously at 322 and 607 MHz, and compare the DM measurements with those obtained through NANOGrav observations with the Green Bank Telescope and Arecibo Observatory at 1400–2300 MHz frequencies. Measured DM values with the GMRT and NANOGrav program show significant offsets for some pulsars, which could be caused by pulse profile evolution between the two frequency bands. In comparison to the predicted DM uncertainties when incorporating these low-frequency data into the NANOGrav data set, we find that higher-precision GMRT data is necessary to provide improved DM measurements. Through the detection and analysis of pulse profile baseline ripple in data on test pulsar B1929+10, we find that, while not important for these data, it may be relevant for other timing data sets. We discuss the possible advantages and challenges of incorporating GMRT data into NANOGrav and International Pulsar Timing Array data sets.