We present a straightforward and efficient method to reduce the mode spacing of a frequency comb based on binary pseudo-random phase modulation of its pulse train. As a proof of concept, we use such a densified comb to perform dual-comb spectroscopy of a long-delay Mach-Zehnder interferometer and a high-quality-factor microresonator with sub-MHz spectral sampling. Since this approach is based on binary phase modulation, it combines all the advantages of other densification techniques: simplicity, single-step implementation, and conservation of the initial comb's power.