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The Burning of Prospero I just ordered will be arriving by tomorrow, so I was also thinking about using Custodian Guards in games.
And I concluded that using psychic is the best way to support the guardians of Golden Throne.
Below is the list I just wrote yesterday. It is not very competitive, but I do not think it is too soft either.
Depending on psychic powers and who goes first, I can either null deploy or start the game with the Custodian Guards and librarians on the board.

1) Primary Detachment : Fist of Medusa Strike Force(Chapter Tactics : Iron Hands)
- Command : Librarius Conclave
Librarian(Mastery Level 2, Terminator Armour, The Gorgon’s Chain, Combi-melta, Force Stave) : 170pts
Librarian(Mastery Level 2, Terminator Armour, Exchange Storm Bolter with Betrayer’s Bane, Force Axe) : 145pts
Librarian(Mastery Level 2, Terminator Armour, Mindforge Stave) : 130pts

- Core : Battle Demi-Company
Terminator Captain(Cataphractii Terminator Armour, Chainfist, Auspex, Shield Eternal) : 190pts (Warlord)
Tactical Squad(1xSergeant : Combi-melta, 4xSpace Marine : Meltagun, Drop Pod : Locator Beacon) : 135pts
Tactical Squad(1xSergeant : Combi-melta, 4xSpace Marine : Meltagun, Drop Pod : Locator Beacon) : 135pts
Tactical Squad(1xSergeant : Combi-grav, 4xSpace Marine : Grav Cannon & Grav Amp, Drop Pod) : 150pts
Land Speeder(2xMulti-melta) : 70pts
Devastator Squad(1xSergeant, 4xSpace Marine : 3xGrav Cannon & Grav Amp, Armorium Cherub, Drop Pod : Locator Beacon) : 225pts

- Auxiliary : Honoured Ancients
Ironclad Dreadnought(2xHeavy Flamer, Seismic Hammer, Power Fist, Ironclad Assault Launcher, Drop Pod : Locator Beacon) : 200pts

2) Golden Legion Task Force
-Elite
Custodian Guard Squad(1xShield-Captain : Guardian Spear, 2xCustodian : 2xGuardian Spear, 1xCustodian : Sentinel Blade & Storm Shield, 1xCustodian : Custodes Vexilla & Storm Shield)
: 310pts

3) Officio Assassinorum Detachment
- Elite
Culexus Assassin : 140pts

Total : 2,000pts

For psychic powers, I believe Sanctic powers are most ideal for supporting Custodian Guard.
Hammerhand is quintessential for buffing S6 guardian spears, whereas gate of infinity is always nice for expensive footsloggers.
Sanctuary improves storm shields' save to 2++, and Vortex of Doom is handy especially when librarians and Custodian Guards arrive via Deep Strike.
The only underwhelming powers are Purge Soul and Cleansing Flame.

1. Your star is gonna be 100% reliant on psychic to survive in most games so the Culexus is iffy.

2. I don't see what the Ironhands are adding to the Custodes, A maxed out Libcon with Tiggy and a GK CAD or Nemesis Strike force would offer more psychic powers which would allow you to get Veil, Sanc, Hammerhand, Endurance, and would guarantee Gate with Draigo. Flavor with dreadknights and call it good.

ERJAK wrote:
1. Your star is gonna be 100% reliant on psychic to survive in most games so the Culexus is iffy.

2. I don't see what the Ironhands are adding to the Custodes, A maxed out Libcon with Tiggy and a GK CAD or Nemesis Strike force would offer more psychic powers which would allow you to get Veil, Sanc, Hammerhand, Endurance, and would guarantee Gate with Draigo. Flavor with dreadknights and call it good.

1. I included Culexus to remove psychic buffs cast on Imperial Knights or Wraithknights. The librarius conclave excels at casting powers, but not at stopping powers. And super-heavies/gargantuan creatures are the most troublesome foes to handle, should they get buffed with invisibility for example.

2. Just like you said, Grey Knights are more compatible with Custodian Guards than the Iron Hands are. It is just that I predominantly use Iron Hands for fluff, and I do not have Grey Knights models. Nor will I be collecting them in near future.