Just dug through the datachain codebase to understand a little more. I think while both projects have a Dataframe interface, they're very different projects!
Datachain seems to operate more on the orchestration layer, running Python libraries such as PIL and requests (for making API calls) and relying on an external database engine (SQLite or BigQuery/Clickhouse) for the actual compute.
Daft is an actual data engine. Essentially, it's "multimodal BigQuery/Clickhouse". We've built out a lot of our own data system functionality such as custom Rust-defined multimodal data structures, kernels to work on multimodal types, a query optimizer, distributed joins etc.
In non-technical terms, I think this means that Datachain really is more of a "DBT" which orchestrates compute over an existing engine, whereas Daft is the actual compute/data engine that runs the workload. A project such as Datachain could actually run on top of Daft, which can handle the compute and I/O operations necessary to execute the requested workload.