You should use NO FILE SYSTEM CACHING on all tablespaces that do not contain LOBs. That is one reason why LOBs should be placed in a separate tablespace when the table is created.
In general, if you have real memory on your database server that always remains unused, then you can increase your bufferpool(s) for better performance, but obviously not larger than the data in the tablespaces assigned to each bufferpool. This has nothing to do with FILE SYSTEM CACHING.