| EP # | TITLE | FIRST AIRED |
| 31 | A SPY FOR A SPY | 10/01/66 |
| 32 | THE ONLY WAY TO DIE | 10/08/66 |
| 33 | STRIKE WHILE THE AGENT IS HOT | 09/24/66 |
| 34 | MAXWELL SMART, ALIAS JIMMY BALLANTINE | 10/15/66 |
| 35 | ANATOMY OF A LOVER | 09/17/66 |
| 36 | KISS OF DEATH | 12/31/66 |
| 37 | CASABLANCA | 10/22/66 |
| 38 | THE GREATEST SPY ON EARTH | 11/19/66 |
| 39 | HOO DONE IT? | 11/05/66 |
| 40 | RUB-A-DUB-DUB... THREE SPIES IN A SUB | 11/12/66 |
| 41 | THE DECOY | 10/29/66 |
| 42 | BRONZEFINGER | 12/03/66 |
| 43 | THE WHOLE TOOTH AND… | 12/24/66 |
| 44 | ISLAND OF THE DARNED | 11/26/66 |
| 45 | PERILS IN A PET SHOP | 12/10/66 |
| 46 | IT TAKES ONE TO KNOW ONE | 01/07/67 |
| 47 | SOMEONE DOWN HERE HATES ME | 01/14/67 |
| 48 | CUTBACK TO CONTROL | 01/21/67 |
| 49 | THE MUMMY | 01/28/67 |
| 50 | THE GIRL FROM KAOS | 02/04/67 |
| 51 | THE MAN FROM YENTA | 02/11/67 |
| 52 | SMART FIT THE BATTLE OF JERICHO | 02/18/67 |
| 53 | WHERE-WHAT-HOW-WHO AM I? | 02/25/67 |
| 54 | HOW TO SUCCEED IN THE SPY BUSINESS | |
| WITHOUT REALLY TRYING | 03/11/67 |
| 55 | THE EXPENDABLE AGENT | 03/04/67 |
| 56 | APPOINTMENT IN SAHARA | 03/25/67 |
| 57 | PUSSYCATS GALORE | 04/01/67 |
| 58 | A MAN CALLED SMART, PART 1 | 04/08/67 |
| 59 | A MAN CALLED SMART, PART 2 | 04/15/67 |
| 60 | A MAN CALLED SMART, PART 3 | 04/22/67 |
| EP # | TITLE | FIRST AIRED |
| 87 | THE IMPOSSIBLE MISSION | 09/21/68 |
| 88 | SNOOPY SMART VS. THE RED BARON | 09/28/68 |
| 89 | CLOSELY WATCHED PLANES | 10/05/68 |
| 90 | SECRET OF SAM VITTORIO | 10/12/68 |
| 91 | DIAMONDS ARE A SPY'S BEST FRIEND | 10/19/68 |
| 92 | THE WORST BEST MAN | 10/26/68 |
| 93 | A TALE OF TWO TAILS | 11/02/68 |
| 94 | THE RETURN OF THE ANCIENT MARINER | 11/09/68 |
| 95 | WITH LOVE AND TWITCHES | 11/16/68 |
| 96 | THE LASER BLAZER | 11/30/68 |
| 97 | THE FARKAS FRACAS | 12/07/68 |
| 98 | TEMPORARILY OUT OF CONTROL | 12/14/68 |
| 99 | SCHWARTZ'S ISLAND | 12/21/68 |
| 100 | ONE NATION, INVISIBLE | 12/28/68 |
| 101 | HOORAY FOR HOLLYWOOD | 01/04/69 |
| 102 | THE DAY THEY RAIDED THE KNIGHTS | 01/11/69 |
| 103 | TEQUILA MOCKINGBIRD | 01/18/69 |
| 104 | I SHOT 86 TODAY | 02/01/69 |
| 105 | ABSORB THE GREEK | 02/08/69 |
| 106 | TO SIRE WITH LOVE, PART 1 | 02/15/69 |
| 107 | TO SIRE WITH LOVE, PART 2 | 02/22/69 |
| 108 | SHOCK IT TO ME | 03/01/69 |
| 109 | LEADSIDE | 03/08/69 |
| 110 | GREER WINDOW | 03/15/69 |
| 111 | THE NOT SO GREAT ESCAPE, PART 1 | 03/15/69 |
| 112 | THE NOT SO GREAT ESCAPE, PART 2 | 03/22/69 |
| EP # | TITLE | FIRST AIRED |
| 113 | PHEASANT UNDER GLASS | 09/26/69 |
| 114 | IRONHAND | 10/03/69 |
| 115 | VALERIE OF THE DOLLS | 10/10/69 |
| 116 | WIDOW OFTEN ANNIE | 10/17/69 |
| 117 | TREASURE OF C. ERROL MADRE | 10/24/69 |
| 118 | SMART FELL ON ALABAMA | 10/31/69 |
| 119 | AND BABY MAKES FOUR, PART 1 | 11/07/69 |
| 120 | AND BABY MAKES FOUR, PART 2 | 11/14/69 |
| 121 | PHYSICIAN IMPOSSIBLE | 11/21/69 |
| 122 | THE APES OF WRATH | 11/28/69 |
| 123 | AGE BEFORE DUTY | 12/05/69 |
| 124 | IS THIS TRIP NECESSARY? | 12/12/69 |
| 125 | ICE STATION SIEGFRIED | 12/19/69 |
| 126 | MOONLIGHTING BECOMES YOU | 01/02/70 |
| 127 | HOUSE OF MAX, PART 1 | 01/09/70 |
| 128 | HOUSE OF MAX, PART 2 | 01/16/70 |
| 129 | REBECCA OF FUNNY-FOLK FARM | 01/23/70 |
| 130 | THE MESS OF ADRIAN LISTENGER | 01/30/70 |
| 131 | WITNESS FOR THE EXECUTION | 02/06/70 |
| 132 | HOW GREEN WAS MY VALET | 02/13/70 |
| 133 | AND ONLY TWO NINETY-NINE | 02/20/70 |
| 134 | SMARTACUS | 02/27/70 |
| 135 | WHAT'S IT ALL ABOUT, ALGIE? | 04/24/70 |
| 136 | HELLO, COLUMBUS; GOODBYE, AMERICA | 05/01/70 |
| 137 | DO I HEAR A VAULTS? | 05/08/70 |
| 138 | I AM CURIOUSLY YELLOW | 05/15/70 |