The frequency-domain mode comb of a Ti:sapphire femtosecond laser centered at 350 THz is broadened to 150 THz (full width at -30 dBc) by self-phase modulation in a single-mode optical fiber. By phase locking continuous-wave lasers to elements of the comb near 1064 and 778 nm, we measure the 104-THz frequency gap between these two lasers with a relative uncertainty of 2.7 x 10(-11) in 1 s.