Titanium‐silicon‐nitride thin films were grown by metallorganic atomic layer deposition (MOALD) using tetrakis(dimethylamido)titanium (TDMAT), ammonia, and silane at 180°C. When the reactants are injected into the reactor in the sequence ofTDMAT pulse,
SiH4
pulse, and
NH3
pulse, the Si content in the Ti‐Si‐N films is saturated at 18 atom %. By changing the supplying sequence in the order of TDMAT,
NH3
, and
SiH4
, the Si content is increased to 21 atom %. The Si content in the films is almost insensitive to the
SiH4
partial pressure over a wide range of 0.27 and 13.3 Pa, because it is self‐limited by the quantity of
SiH4
molecules absorbed on the film surface. By utilizing these inherent characteristics of MOALD, digital control of Si content in Ti‐Si‐N thin film is possible by controlling the number of
SiH4
pulses during film deposition. The MOALD Ti‐Si‐N films have almost 100% step coverage on a 0.3 μm diam hole with an aspect ratio of 10:1. MOALD is considered to be a promising deposition method for less than 10 nm thick Ti‐Si‐N films as a Cu diffusion barrier film. © 2000 The Electrochemical Society. All rights reserved.