Tetrapod-shaped maghemite nanocrystals are synthesized by manipulating the decomposition of iron pentacarbonyl in a ternary surfactant mixture under mild thermal conditions. Adjustment of the reaction parameters allows for the systematic tuning of both the width and the length of the tetrapod arms, which grow preferentially along the 111 easy axis direction. Such degree of control leads to modulation of the magnetic behavior of the nanocrystals, which evolves systematically as their surface magnetization phase and shape anisotropy are progressively increased.