Durable, sensitive and wearable electronics are highly desirable for monitoring everything from vital signs to athletic performance. However, electronic textiles with excellent functions, stability, comfort, and durability against washing/rubbing remain a big challenge. Herein, a coating containing nanocomposites of polyaniline (PANI) with nanodiamond (ND) was applied to the surface of wool fabrics through an in situ polymerization technique. The nanocomposite fabrics with PANI-ND demonstrated high sensitivity, enhanced durability, and excellent mechanical properties without compromising the inherent properties of textiles such as comfort and breathability. Wool fabrics were treated with aniline, aniline-ND, and aniline-boron doped ND (BDND) to investigate the molecular interaction between ND/BDND and PANI and their effects on the final properties, such as comfort, mechanical and electrochemical properties of the treated fabric. The PANI-ND coated fabrics showed sheet resistances below 10 kΩ/sq and up to a 2-fold decrease in response to monotonically increasing and cyclic mechanical strains compared with the PANI-coated fabric. Wool fabric coated with PANI-ND is a sensitive sensor that can withstand strain up to 100%, which is remarkable for delicate fibers. The developed sensor can detect human motion, such as bending of a finger to different angles. The moisture properties of the fabric coated with PANI-ND improved significantly along with durability against washing and abrasion without affecting its breathability. This work provides insights into developing highly sensitive multifunctional electronic textiles (such as wearable sensors) without compromising the intrinsic properties of textiles.