LS seems to not be claiming any security promise on Linux because it can't make any guarantees given eBPF limitations. But the entire purpose is different and there is very little overlap in my view. PiHole is entirely (I think?) just applying the blocklist made easy. LS allows you to build the blocklist in real time.

I would guess that to the extent the blocklists include things that are loaded by applications and not websites, they are almost entirely built by users of something like LittleSnitch or OpenSnitch. This is also entirely doable with wireshark logs, but I think that requires more infrastructure to build into usable lists.