This problem has been much studied. While it may be difficult to define what 'best' is, there is a very efficient one already in existence, and that's PGP Words. This method was designed for transmitting long binary keys over a voice link, each word encoding a whole 8 bit byte.
It addresses a number of problems you probably haven't thought of, like reliability over a voice link. What happens if a word is missed, or a repetition for clarity is mistaken as an actual repetition or, reading from a long list, two words get swapped?
With 8 bits per word, you would normally require 256 words. The system is more sophisticated than that, and uses 512 words, an 'even' table of two syllable words, and an 'odd' table with three syllables, that are used alternately. That way, a missed or repeated word, or two swapped words, can be immediately spotted as an error.
Here are the first few and last few, from the wikipedia article linked above. The whole table can be printed on a single sheet of A4. They are in alphabetical order to aid the receiver. Obviously the list is optimised for English. Speakers of other languages may prefer a different list.
Hex Even Word Odd Word
--- --------- --------
00 aardvark adroitness
01 absurd adviser
02 accrue aftermath
03 acme aggregate
04 adrift alkali
.. ...... .......
FB watchword Wichita
FC wayside Wilmington
FD willow Wyoming
FE woodlark yesteryear
FF Zulu Yucatan
Quote from the wikipedia article
The PGP Word List was designed in 1995 by Patrick Juola, a computational linguist, and Philip Zimmermann, creator of PGP. The words were carefully chosen for their phonetic distinctiveness, using genetic algorithms to select lists of words that had optimum separations in phoneme space. The candidate word lists were randomly drawn from Grady Ward's Moby Pronunciator list as raw material for the search, successively refined by the genetic algorithms. The automated search converged to an optimized solution in about 40 hours on a DEC Alpha, a particularly fast machine in that era.
An alternative for a 4 bit nybble per word is simply to use the hex alphabet, perhaps using the ICAO/NATO pronunciation, 'zero' to 'niner' then 'alpha' through to 'foxtrot'. There are more than 16 further letters left if needed for even/odd coding. Whether the complexity of the 512 words needed for doubling the throughput with PGP words is warranted against the simplicity of hex begs the question of how you define 'best', what factors in the setup or operation of the communication are important.
You could get even higher efficiency by using more bits per word. 12 bits would need a 4096/8192 long dictionary. This would sacrifice much of the hard-won inter-word phonetic distance of the PGP scheme, so would require a higher fidelity voice channel, and more careful speakers.
Noting ruakh's comment, it's worth looking at the speed of the channel. His estimate is two seconds per word, which would probably be quite good for untrained users. That's 4 bits/s. If we compare that with Morse code, the minimum speed required by the FCC to grant a radio operator's license used to be 16 five-letter code groups per minute, which very roughly equates to about 8 bits/s.
The difference between the two systems is that Morse Code requires training. I couldn't transcribe Morse, at any speed, without a lot of practice, and probably some tuition as well. Many English speakers could transcribe those words without practice, but what about those with a limited vocabulary, or English as a second language, or speakers of other languages? PGP words is not really training-free, if it's to be used by any human at all. It's only ready-to-go if used by people like those who invented it, educated fluent English speakers, being a programmer would help as well. It's probably a skill that's easier to pick up than Morse though.
With speed in mind, it might be worth reviewing the performance of hexadecimal via ICAO pronunciation. While a word every two seconds would be good going for recording a PGP word manually, I think hexadecimal could be done at easily twice that rate, transcribing as you go, making the bit rate of the two methods equivalent.
Clearly a lot of other assumptions about the training or experience of users, the setup costs, the quality of the audio link, have to be defined before the best system can be determined.