We present a detailed low-temperature investigation of the statics and dynamics of the anions and methyl groups in the organic conductors (TMTSF) 2 PF 6 and (TMTSF) 2 AsF 6 (TMTSF: tetramethyl-tetraselenafulvalene). The 4 K neutron-scattering structure refinement of the fully deuterated (TMTSF) 2 PF 6 -D12 salt allows locating precisely the methyl groups at 4 K. This structure is compared to the one of the fully hydrogenated (TMTSF) 2 PF 6 -H12 salt previously determined at the same temperature. Surprisingly, it is found that deuteration corresponds to the application of a negative pressure of 5 × 10 2 MPa to the H12 salt. Accurate measurements of the Bragg intensity show anomalous thermal variations at low temperature both in the deuterated PF 6 and AsF 6 salts. Two different thermal behaviors have been distinguished. Small Bragg-angle measurements reflect the presence of low-frequency modes at characteristic energies θ E = 8.3 K and θ E = 6.7 K for the PF 6 -D12 and AsF 6 -D12 salts, respectively. These modes correspond to the low-temperature methyl group motion. Large Bragg-angle measurements evidence an unexpected structural change around 55 K, which probably corresponds to the linkage of the anions to the methyl groups via the formation of F. . .D-CD 2 bonds observed in the 4 K structural refinement. Finally we show that the thermal expansion coefficient of (TMTSF) 2 PF 6 is dominated by the librational motion of the PF 6 units. We quantitatively analyze the low-temperature variation of the lattice expansion via the contribution of Einstein oscillators, which allows us to determine for the first time the characteristic frequency of the PF 6 librations: θ E ≈ 50 K and θ E = 76 K for the PF 6 -D12 and PF 6 -H12 salts, respectively.