Nine compounds containing fluorine or chlorine atoms in the lateral position in the rigid core with a chiral terminal octyloxy-chain were synthesized mainly using Suzuki-Miyaura coupling, Mitsunobu, hydrogenation, and esterification reactions. New compounds were investigated using polarized optical microscopy (POM), differential scanning calorimetry (DSC), spectrophotometry, and electro-optical methods. A computational analysis of the effect of lateral substitution by halogen atoms on the phenyl ring on the dipole moment of the compound was provided and discussed. The designed compounds exhibit a wide temperature range of the ferroelectric phase (>40.0 °C), a low melting point (in most cases below 50.0 °C), low melting enthalpy (around 10.0–20.0 kJ/mol), a short helical pitch (in most cases below 200 nm at room temperature) and high tilt angle that ensures a cone angle of up to 90°; all those properties make them of great potential for the deformed helix ferroelectric (DHF) mode. Revealed features allow synthesized compounds in fully integrated polarization-based photonic transducers to have excellent linearity and the highest sensitivity observed in ferroelectric liquid crystals for DHF mode. For the first time, the DHF effect was reached for the single molecule FLC material in a broad temperature range down to 38 °C. These findings pave the way for a new class of optical sensors for, among others, industrial monitoring networks and brain/machine interfaces with unprecedented performance.