This phrase refers back to the preceding section, so it needs to be understood in context. The speaker has been talking about the joy he derives from nature, being in nature, and hearing the voice of the river, the "sylvan Wye," in every aspect of nature as he gazes upon it. The speaker also talks about the pureness with which children look upon and take joy in nature, and he wishes that he had not lost that fervor and zeal.
However, he describes himself still as "a worshipper of nature." This is where the phrase you have identified comes in. As a worshipper, the speaker has come to this spot, a few miles above Tintern Abbey, "unwearied in that service"—that is, still a dedicated worshipper of nature who has not become tired of serving nature in that way. The word "service" is carefully chosen, as it suggests a church service,...
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where attendees would worship God without becoming tired of that devotion. In the same way, the speaker has been a longtime devotee of nature.
William Wordsworth was inspired to write Lines Composed A Few Miles Above Tintern Abbey after"a long absence" of five years from the banks of the river Wye of which he has pleasant memories and it makes him feel "tranquil restoration." These memories have enabled him to manage the challenges of life as "the heavy and the weary weight / Of all this unintelligible world, Is lightened."
Wordsworth admits to having a more enlightened and philosophical approach to life than he used to and he cherishes this opportunity to spend time with his sister as "we stood together."
The term "unwearied in that service" refers to a tradesman, for example, who is "in service;" in other words, regarding his occupation in which he remains content never becoming bored or dissatisfied. In this context, as "A worshipper of Nature," Wordsworth will remain "Unwearied in that service" as he will never tire of the beauty and wonder of nature. Even the absence of five years cannot reduce its beauty or the importance of the place in his memory, made all the more exceptional by his sister's presence there .
What does "unwearied in that service" mean in "Tintern Abbey"?
These lines come in the final stanza of this lengthy meditation about nature and man's relationship with it. The phrase "unwearied in that service" is used by the speaker to describe his own self and his relationship to nature, and how, for his entire life, he has been a follower of nature. Even though he has not returned to Tintern Abbey for a long time, he still reflects that his entire life has been led as an acolyte of nature, as the quote in its entirety reveals:
...and that I, so long
A worshipper of Nature, hither came,
Unwearied in that service.
It is interesting that Wordsworth chooses to describe himself as a "worshipper of Nature," revealing how, in his Romantic view, nature is not something to be scientifically and dispassionately considered, but it is something that should engage our emotions, our awe and wonder. The phrase "unwearied in that service" reveals more about the kind of relationship that Wordsworth has with nature. Although he is a self-confessed "worshipper," this relationship is not in any way tiring or exhausting. After all, years after coming to Tintern Abbey in the first place, he is still happy to describe himself as a "worshipper of Nature." Rather, this relationship with nature is something that empowers him and fulfills him.