This work brings together diamond anvil cell techniques, vibrational spectroscopies, and complementary lattice dynamics calculations to investigate pressure-induced local lattice distortions in alpha-Co[N(CN)(2)](2). Analysis of mode behavior and displacement patterns reveals a series of pressure-driven transitions that modify the CoN6 counter-rotations, distort the octahedra, and flatten the C-N-ax-C linkages. These local lattice distortions may be responsible for the low temperature magnetic crossover. We also discuss prospects for negative thermal expansion and show that there is not a straightforward low pressure pathway between the pink alpha and blue beta ambient pressure phases of Co[N(CN)(2)](2).