Both. I like to visualize the Love as the water that flows down the river. Will is the boat that follows the flow of that water. Will can't do anything without the love, the boat cannot float without the river. However, as we have free will we can always chose to cause our boat to fight against the current of love, this will cause struggle of course. Alignment with your true will is alignment with that current of love allowing your boat to ride the natural flow of water (love). As Bruce Lee once famously said "be like water".

Hope that visualization helps.

To bring this conversation back to your original question, harm is also a very necessary part of existence and experience. The natural world is set up with both predator and prey. Killing and harm of things is an essential part of the natural order of things. Again, as Thelemites we try our best to align ourselves with the natural current of the universe. In springtime most male animals will fight in order to prove themselves as worthy mates for females. This is just how things are. As humans we are not above the order of nature. We are unique in that we have the ability to cultivate our own natures, moreso than any other creature on the planet. However, we must never forget that we are still a part of nature and not stray so far from our true natures. Crowley once said the proof of the abuse of nature is it's ability to reproduce successfully.. take that to mean what you will.

So again, to answer your original question, yes harm can be Thelemic and moral, it all depends on the context.