Using the data acquired in the Time To Spill (TTS) mode for long gamma-ray bursts (GRBs) collected by the Burst and Transient Source Experiment on board the Compton Gamma Ray Observatory (BATSE/CGRO), we have carefully measured spectral lags in time between the low (25-55 keV) and high (110-320 keV) energy bands of individual pulses contained in 64 multi-peak GRBs. We find that the temporal lead by higher-energy gamma-ray photons (i.e., positive lags) is the norm in this selected sample set of long GRBs. While relatively few in number, some pulses of several long GRBs do show negative lags. This distribution of spectral lags in long GRBs is in contrast to that in short GRBs. This apparent difference poses challenges and constraints on the physical mechanism(s) of producing long and short GRBs. The relation between the pulse peak count rates and the spectral lags is also examined. Observationally, there seems to be no clear evidence for systematic spectral lag-luminosity connection for pulses within a given long GRB.