Every once in a while, my iPod does a spectacular job at shuffling the perfect set of songs. Is there any way to save this sequence to a playlist so I can replay it again in the future?
You have two options.
1. On-the-road compatible, but not so user-friendy
They will be kept in sort order, and the playlist will be synced to iTunes for future use.
2. Much easier, but with listening limitations
The only problem with this solution is that if you listen to one of the songs that were in your set, it will have its Last played field updated, and won't be in the proper place… So this solution is usable only if you can sync pretty quickly after listening to the set, or can remember a few songs' positions, or if you avoid listening to them altogether before the next sync.
From any list of songs in iTunes (like for example, when you're on iTunes DJ) you can select the range of songs by clicking while holding the Shift key. Once all songs are highlighted you can go the File menu and select New Playlist From Selection. A new playlist will be shown at the bottom of the Playlist section containing the exact same song selection and ordering. Hope this helps.
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But there is laborous workaround: If you don't use star rating normaly or using it but never use one star (or two) then go through every song that was playing during shuffle and star them.
After that sync to iTunes, create a Smart Playlist and sort it by the last played column. If you need to sync it back to iPod choose Copy to Play Order. More on this here.