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All great - the orchestral set is a real bonus. If only the final mvt of No. 4 delivered on what goes before, but it doesn't. MTT's slower, grander performance with the Chicago orchestra does it much better.
I by no means question his contributions to the field, but try as I might to not have to I need literally force myself to listen to his works. A rule of thumb is that the fewer instruments involved the better. Certain of his songs and choral works are very good if not memorable (for example, "They Are There!"), and E. Power Biggs playing "Variations on 'America'" can't be topped.
His Second Symphony would be the gentlest introduction to Ives' orchestral works, but when you listen to more by him you should recognize that's not quite the Ives you came for. Instead, his Third Symphony gets my vote. On this disc, the Fugue and Finale for the "reali[z]ed and edited" Performance Score of his Fourth Symphony also entice somewhat. Anything else is an acquired taste.
I also by no means say that virtuosity isn't an utter necessity to perform anything by Ives. Maestro Davis and the Melbourne have and display that throughout, and they've helped me last through the orchestral works of Ives I've heard in one sitting. May you appreciate those better.