We explore and demonstrate the use of phase-modulated ultrafast laser pulses for controlling nonlinear optical processes in large molecules, proteins, and solid materials. Our experiments illustrate that in condensed phases, when spectra are broad, the spectrum of the nth-order electric field, determined by multiphoton intrapulse interference, plays a major role in controlling multiphoton excitation. These findings determine key parameters (amplitude, period, and symmetry of the phase function) for coherent femtosecond laser control in condensed phases.