Observations of optical interstellar absorption lines of Ti II, Ca II, and/or Na I acquired at an instrumental resolution typically of 5.6 km/s are reported for 29 stars. The data were recorded primarily with a Digicon detector and achieve 2 sigma detection limits generally near an equivalent width of 1 mA. The primary purpose of the observations is, in combination with previously published data, to provide a comprehensive, high-sensitivity survey of Ti II, Ca II, and Na I absorption at all velocities, toward 41 stars for which a correspondingly complete survey of certain ultraviolet interstellar lines also is available. New high-velocity optical interstellar lines at /v(LSR)/ greater than about 25 km/s are found toward four of the 29 stars.