A liquid crystalline elastomer (LCE) exhibiting a chiral smectic C phase (S-c* phase) was synthesized and macroscopically ordered by mechanical deformations. The elastomer displays a permanent noncentrosymmetric structure and is therefore suitable for second harmonic generation (SHG) without applying external electrical poling fields. Using the Maker fringe experiment, the three largest nonlinear optical coefficients d(ig) were measured and the temperature dependence observed. This liquid-crystal system represents a new class of material for nonlinear optics.