I agree that it is almost impossible to pick just one Ray Bradbury science fiction story as "the greatest". However, two personal favorites that immediately come to mind are "There Will Come Soft Rains" and "All Summer in A Day". Both are sad, poignant, and (at least for me) unforgettable.
This is a very good question, because many people think Ray was mainly a science fiction writer, while he often said he wasn't a science fiction writer at all (except for Fahrenheit 451, which he admitted was SF). The truth is somewhere in between. Ray did write science fiction — a lot of it — during the 1940s, but after Fahrenheit 451 he wrote virtually no new SF.
So what was the best of his science fiction period?
In all probability, Ray's best science fiction story is "And the Rock Cried Out".
If you absolutely forced me to name just one SF story by him, that's the one I'd name.
However, there are other very strong contenders: "There Will Come Soft Rains", "A Sound of Thunder", "The Veldt", and "The Fog Horn". "The Fireman" (the shorter version of Fahrenheit 451), must be considered as well.
And don't forget the story that was for many years my favorite Ray Bradbury story: "Frost and Fire". The first few pages are as good as anything I've mentioned here, although the story is a bit more ordinary towards the end.
"The Long Rain" and "All Summer in a Day" (his two Venus stories) are good too. There are others, but I'll stop there!
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He was a writer who wrote science fiction, and speculative fiction, and fantasy, and horror, and, well, he just wrote. He was a writer. As a kid, I welcomed his diversity, because I never would have read a book like Dandelion Wine if Bradbury hadn't already hooked me with his science fiction and fantasy.
A favorite not mentioned yet in this thread in The Golden Apples of the Sun, a captivating tale masterfully told by Bradbury. He could pull us in with the turn of a phrase, or take a collection of stories and make them something greater when brought together in the Illustrated Man. "It was a warm afternoon in September when I first met the Illustrated Man." From the first line, he captivates you, draws you in, wanting to know more.
Mike, I know exactly what you mean. I first read Ray when I was in seventh grade. I had taken out a couple of Robert Heinlein science fiction novels from my school library, and was disappointed to learn those were the only two Heinlein books my school library had. A very wise librarian pulled a book off the shelf, handed it to me, and said, "Why don't you take out this one? I think you'll like it." I went home, sat under a tree in the backyard of my parent's house, and began to read. The book was THE GOLDEN APPLES OF THE SUN. I couldn't put the book down. I still remember thinking: "Rocketships! Dinosaurs! Baseball! All the thing I love. This writer must have written this book just for me." I imagine a lot of Ray's readers feel the same way. I've been hooked on Ray's writing ever since. I once told the foregoing story to Ray and added, "I don't know what Isaac Newton felt like when that apple hit him in the head while sitting under a tree, but it was probably the same way I felt sitting under that tree in my backyard reading your stories."
Richard, another one of his fine stories can be found in The Golden Apples of the Sun collection -- "The Foghorn," which was originally published as “The Beast from 20,000 Fathoms.” It's as much about loneliness and the modern world meeting the past as it is about monsters. I read it again a month or so back and it was better than I had remembered, or perhaps I have a different appreciation and understanding when I'm older compared to my younger self. It's not a science fiction story, but it reminds me there are so many great Bradbury stories that I have difficulty narrowing it to but a few.