Chuang Tzu and Heidegger both emphasise the virtue of 'spontaneity' - a sort of mindful responsiveness to things as they are. It's this notion, I suspect, that is the best bet for helping to make some sense of talk about harmony or unity with nature.
The focus of environmental ethics should indeed be on the virtues and how these inform our relationship to natural environments.
Gardening is an excellent example of a practice to which, as Alasdair MacIntyre puts it, certain virtues are 'internal'. Good gardening requires a certain goodness on the part of the gardener: care, humility, patience, and respect, for example.
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