Yes, you can. There isn't a "disk controller" in a SCSI interface, at least not in the IDE sense. The limitation is with the Operating System.

Systems before 7.5.5 support a drive no larger than 4GB, but Appleshare won't support networked drives more than 2GB.

System 7.5.5 and up support partitions of up to two terabytes. If you had a two terabyte partition you would get extremely large minimum file sizes, unless you've got HFS+ on 8.1 and up.

Systems 9.1 and newer can have files larger than 2GB but that doesn't apply to a 68K Mac which can only use up to 8.1, so you're stuck with a max file size of 2GB on 68K